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  • 1.
    Adeniyi, Omotayo
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Osmanaj, Blerina
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Department of Chemistry, University of Prishtina, Prishtina, Republic of Kosovo.
    Manavalan, Gopinathan
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Industrial Chemistry and Reaction Engineering, Johan Gadolin Process Chemistry Centre, Åbo Akademi University, Åbo-Turku, Finland.
    Berisha, Avni
    Department of Chemistry, University of Prishtina, Prishtina, Republic of Kosovo.
    Tesfalidet, Solomon
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Reagentless impedimetric immunosensor for monitoring of methotrexate in human blood serum using multiwalled carbon nanotube@polypyrrole/polytyramine film electrode2024Ingår i: Talanta: The International Journal of Pure and Applied Analytical Chemistry, ISSN 0039-9140, E-ISSN 1873-3573, Vol. 268, nr Part 1, artikel-id 125316Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Ensuring effective monitoring of methotrexate (MTX) levels in the bloodstream of cancer patients undergoing high-dose methotrexate chemotherapy is crucial to prevent potentially harmful side effects. However, the absence of portable analytical devices suitable for point-of-care bedside monitoring has presented a significant obstacle to achieving real-time MTX monitoring. In this study, we developed an impedimetric immunosensor that doesn't require reagents for measuring MTX levels in undiluted human blood serum. This reagentless approach simplifies the assay process, enabling rapid and straightforward MTX quantification. The immunosensor transducer was fabricated by electrodepositing conductive network of porous multiwalled carbon nanotube@polypyrrole/polytyramine on screen-printed gold microchip electrode (SP–Au/MWCNT70@PPy-PTA). Polyclonal anti-MTX antibodies were immobilized on the film, acting as the immunorecognition element. Non-specific binding was prevented by blocking the transducer interface with denatured bovine serum albumin (dBSA) fibrils, resulting in SP-Au/MWCNT70@PPy-PTA/anti-MTXAb|dBSA film electrode. When MTX binds to the SP-Au/MWCNT70@PPy-PTA/anti-MTXAb|dBSA interface, the film conductance and electron transfer resistance changes. This conductivity attenuation allows for electrochemical impedimetric signal transduction without a redox-probe solution. The electrochemical impedance spectroscopy (EIS) results showed increased charge transfer resistance and phase angle as MTX concentrations increased. The SP-Au/MWCNT70@PPy-PTA/anti-MTXAb|dBSA demonstrated high sensitivity, with a linear response from 0.02 to 20.0 μM and a detection limit of 1.93 nM. The detection limit was 50 times lower than the intended safe level of MTX in human serum. The immunosensor exhibited minimal cross-reactivity with endogenous MTX analogs and serum proteins. The SP-Au/MWCNT70@PPy-PTA/anti-MTXAb|dBSA immunosensor presents a simple and rapid method for therapeutic drug monitoring compared to traditional immunoassay systems.

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  • 2.
    Adeniyi, Omotayo
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Osmanaj, Blerina
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Department of Chemistry, University of Prishtina, 10000 Prishtina, Kosovo.
    Manavalan, Gopinathan
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Samikannu, Ajaikumar
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Industrial Chemistry and Reaction Engineering, Johan Gadolin Process Chemistry Centre, Åbo Akademi University, Åbo-Turku, 20500, Finland.
    Avni, Berisah
    Department of Chemistry, University of Prishtina, 10000 Prishtina, Kosovo.
    Boily, Jean-Francois
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Tesfalidet, Solomon
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Engineering of layered iron vanadate nanostructure for electrocatalysis: simultaneous detection of methotrexate and folinic acid in blood serum2023Ingår i: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, artikel-id 142538Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    In this study, nanostructure kazakhstanite-like iron vanadate (FexV3xOy.H2O) was synthesized and calcined at different temperatures (100-800 °C) in a nitrogen atmosphere. The material was used to modify screen-printed carbon electrodes to achieve an electrocatalytic effect on the surface. The relationship between calcination conditions and the catalytic performance of the electrode towards the oxidation of chemotherapeutic drugs, including methotrexate (MTX) and folinic acid (FA), was studied. Various spectroscopic, microscopic, and electrochemical methods were used to characterize the synthesized materials. The results show that calcination induces changes in the electronic structure, nanostructure morphology, electroactive surface area, and electrocatalytic performance of the material. Screen-printed carbon electrode modified with FexV3xOy calcinated at 450 °C (SPC/FexV3xOy-450) was used to develop a voltammetric sensor for the determination of MTX and FA in blood serum. The response of the SPC/FexV3xOy-450 towards the electrooxidation of MTX and FA was the highest in comparison to the bare SPC and SPC/FexV3xOy calcined at other temperatures. The SPC/FexV3xOy-450 exhibited a linear relationship over a wide concentration range: 0.005-200 µM for MTX and 0.05-200 µM for FA. The detection limit was 2.85 nM for MTX and 7.79 nM for FA. Compared to conventional methods, the SPC/FexV3xOy-450 sensor had a short response time (5 min) for simultaneous detection of MTX and FA without signal interferences from coexisting electroactive compounds. The accurate and precise determination of MTX in the presence of FA confirmed the potential clinical applications of SPC/FexV3xOy-450 for therapeutic drug monitoring during chemotherapy.

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  • 3. Aguilera, Adriana Freites
    et al.
    Tolvanen, Pasi
    Heredia, Shuyana
    Muñoz, Marta González
    Samson, Tina
    Oger, Adrien
    Verove, Antoine
    Eränen, Kari
    Leveneur, Sebastien
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Industrial Chemistry & Reaction Engineering, Department of Chemical Engineering, Johan Gadolin Process Chemistry Centre, Åbo Akademi University, Åbo-Turku, Finland.
    Salmi, Tapio
    Epoxidation of fatty acids and vegetable oils assisted by microwaves catalyzed by a cation exchange resin2018Ingår i: Industrial & Engineering Chemistry Research, ISSN 0888-5885, E-ISSN 1520-5045, Vol. 57, nr 11, s. 3876-3886Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Epoxidation of oleic acid and cottonseed oil was conducted in a semibatch reactor with in-situ-formed percarboxylic acid (peracetic acid or perpropionic acid), using hydrogen peroxide as an oxidizing agent and carboxylic acid (acetic acid or propionic acid) as oxygen carriers. Amberlite IR-120 was implemented as the catalyst. The system was comprised of a loop reactor, where the mixture was pumped through a single-mode cavity in which microwave irradiation was introduced. A heat exchanger was integrated into the system to replace microwave heating, to compare the results obtained via microwave heating versus conventional heating. The catalyst loading effect was studied, as well as the influence of microwave irradiation and the implementation of the SpinChem rotating bed reactor (RBR), in hopes of decreasing the influence of the internal mass transfer. The application of microwave irradiation results in an improvement of the reaction yield in the absence of a catalyst.

  • 4. Aguilera, Adriana Freites
    et al.
    Tolvanen, Pasi
    Oger, Adrien
    Eränen, Kari
    Leveneur, Sébastien
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Department of Chemical Engineering, Johan Gadolin Process Chemistry Centre, Åbo Akademi University, Turku-Åbo, Finland.
    Salmi, Tapio
    Screening of ion exchange resin catalysts for epoxidation of oleic acid under the influence of conventional and microwave heating2019Ingår i: Journal of chemical technology and biotechnology (1986), ISSN 0268-2575, E-ISSN 1097-4660, Vol. 94, nr 9, s. 3020-3031Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Background: For many chemical systems, it is of great importance to find a durable, active and efficient catalyst that improves the process performance. Epoxidation of oleic acid with peracetic acid (Prilezhaev oxidation) was carried out in an isothermal loop reactor in the presence of heterogeneous catalysts. The kinetic experiments conducted under microwave heating (MW) were compared with identical experiments carried out under conventional (conductive/convective) heating. Extensive screening of heterogeneous catalysts was conducted and the influence of microwave irradiation on the reaction kinetics was studied. Several ion exchange resins were screened to explore their applicability and activity in the epoxidation of oleic acid. The perhydrolysis reaction (peracetic acid formed in situ from acetic acid and H2O2) was promoted with the use of various solid acid catalysts: Amberlite IR-120, Amberlyst 15, Smopex®, Dowex 50x8-100, Dowex 50x8-50, Dowex 50x2-100 and Nafion™.

    Results: From the selected group of catalysts, Dowex 50-x8100 and Dowex 50x8-50 produced the highest yield of epoxidized oil. Only minor differences in the reactant conversion and the product yield were found in the experiments carried out under microwave exposure compared to the conventionally heated experiments in the presence of several ion exchange resins.

    Conclusions: The catalytic effect was much more prominent than the microwave effect, because the solid acid catalysts enhanced the slow step of the process, the perhydrolysis of acetic acid. The catalytic effect was very dominant and a considerable improvement of the oleic acid conversion and the epoxide yield was observed in the presence of the top-performing catalysts.

  • 5.
    Ahlkvist, Johan
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Ajaikumar, Samikannu
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Larsson, William
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    One-pot catalytic conversion of Nordic pulp media into green platform chemicals2013Ingår i: Applied Catalysis A: General, ISSN 0926-860X, E-ISSN 1873-3875, Vol. 454, s. 21-29Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    In this paper, both sulphite and sulphate (Kraft) cellulose from Nordic pulp mills were used as raw materials in the catalytic one-pot synthesis of green platform chemicals, levulinic and formic acids, respectively. The catalyst of choice was a macro-porous, cationic ion-exchange resin, Amberlyst 70. The optimal reaction conditions were determined and the influence of various gas atmospheres was investigated. The maximum yields of 53% formic acid and 57% of levulinic acid were separately obtained in a straight-forward conversion system only containing cellulose, water and the heterogeneous catalyst. The concept introduces a one-pot procedure providing a feasible route to green platform chemicals obtained via conversion of coniferous soft wood pulp to levulinic and formic acids, respectively.

  • 6.
    Ahlkvist, Johan
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Mäki-Arvela, Päivi
    Åbo Akademi.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Åbo Akademi University, Process Chemistry Centre, Åbo Akademi University, Industrial Chemistry & Reaction Engineering., Finland.
    Macro-molecules as a source of levulinic acid2014Ingår i: International Review of Chemical Engineering, ISSN 2035-1755, Vol. 16, nr 1, s. 44-58Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    The production of levulinic acid from biomass and macromolecules has been reviewed. It was concluded that the most important parameters in the one-pot hydrolysis of biomass, also including dehydration of glucose to hydroxymethylfurfural as well as its further rehydration to formic and levulinic acids, respectively, are the reaction temperature, initial reactant concentration, acid type as well as the raw material applied. The theoretical maximum yield can hardly be obtained due to formation of humins. Further, the optimum reaction conditions as well as the influence of the catalyst and biomass type are also discussed.

  • 7.
    Ahlkvist, Johan
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Samikannu, Ajaikumar
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Larsson, William
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Wärnå, Johan
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University, Åbo, Finland.
    Salmi, Tapio
    Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University, Åbo, Finland.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University, Åbo, Finland.
    Reaction Network upon One-pot Catalytic Conversion of Pulp2013Ingår i: / [ed] Sauro Pierucci, Jiří J. Klemeš, AIDIC - associazione italiana di ingegneria chimica, 2013, Vol. 32, s. 649-654Konferensbidrag (Refereegranskat)
    Abstract [en]

    Nordic sulphite and sulphate (Kraft) cellulose originating from Nordic pulp mills were used as raw materials in the catalytic synthesis of green platform chemicals, levulinic and formic acids, respectively. The catalyst of choice used in this study was a macro-porous, cationic ion-exchange resin Amberlyst 70 for which the optimal reaction conditions leading to best yields were determined. For this system, maximum yields of 53 mol-% and 57 mol-% were obtained for formic and levulinic acid, respectively. The reaction network of the various chemical species involved was investigated and a simple mechanistic approach involving first order reaction kinetics was developed. The prototype model was able to describe the behaviour of the system in a satisfactory manner.

  • 8.
    Ahlkvist, Johan
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Samikannu, Ajaikumar
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Catalytic conversion of lignocellulosic materials2010Konferensbidrag (Övrigt vetenskapligt)
  • 9.
    Ahlkvist, Johan
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Wärnå, Johan
    Åbo Akademi.
    Salmi, Tapio
    Åbo Akademi.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Experimental and Kinetic Modelling Studies upon Conversion of Nordic Pulp into Levulinic AcidManuskript (preprint) (Övrigt vetenskapligt)
    Abstract [en]

    In this paper, sulphite cellulose from a Swedish pulp mill was applied as the raw material upon catalytic, one-pot synthesis of green platform chemicals – levulinic and formic acids. Cationic ion-exchange resin, Amberlyst 70, was the catalyst of choice and the optimal reaction conditions leading to best yields were determined. The kinetic experiments were performed in a temperature range of 180–200 °C and an initial substrate concentration regime ranging from 0.7 to 6.0 wt %. For this system, maximum theoretical yields of around 59 mol % and 68 mol % were obtained for formic and levulinic acid, respectively. These yields were achieved at a reaction temperature of 180 °C and an initial cellulose intake of 0.7 wt %. A simplified reaction network of the various chemical species involved was investigated and a mechanistic approach involving first order reaction kinetics was developed. The model was able to describe the behaviour of the system in a satisfactory manner (degree of explanation 97.8 %). Since the solid catalyst proved to exhibit good mechanical strength under the experimental conditions applied here, the concept introduces a one-pot procedure providing a route to green platform chemicals from coniferous soft wood pulp to produce levulinic and formic acids, respectively.

  • 10.
    Ahlkvist, Johan
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Wärnå, Johan
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University,Turku, Finland.
    Salmi, Tapio
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University,Turku, Finland.
    Heterogeneously catalyzed conversion of nordic pulp to levulinic and formic acids2016Ingår i: Reaction Kinetics, Mechanisms and Catalysis, ISSN 1878-5190, E-ISSN 1878-5204, Vol. 119, nr 2, s. 415-427Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Herein, one-pot conversion of cellulose to platform chemicals, formic and levulinic acids was demonstrated. The catalyst selected was an affordable, acidic ion-exchange resin, Amberlyst 70, whereas the cellulose used was sulfite cellulose delivered by a Swedish pulp mill. Furthermore, in an attempt to better understand the complex hydrolysis network of the polysaccharide, kinetic experiments were carried out to pinpoint the optimal reaction conditions with an initial substrate concentration of 0.7–6.0 wt% and a temperature range of 180–200 °C. Higher temperatures could not be used due to the limitations in the thermal stability of the catalyst. Overall, maximum theoretical yields of 59 and 68 mol% were obtained for formic and levulinic acid, respectively. The parameters allowing for the best performance were reaction temperature of 180 °C and initial cellulose concentration of 0.7 wt%. After studying the behavior of the system, a simplified reaction network in line with a mechanistic approach was developed and found to follow first order reaction kinetics. A satisfactory fit of the model to the experimental data was achieved (97.8 % degree of explanation). The catalyst chosen exhibited good mechanical strength under the experimental conditions and thus, a route providing green platform chemicals from soft wood pulp from coniferous trees (mixture of Scots Pine and Norway Spruce) was demonstrated.

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  • 11. Aid, T.
    et al.
    Hyvarinen, S.
    Vaher, M.
    Koel, M.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Johan Gadolin Process Chemistry Centre, Åbo Akademi University, Åbo-Turku, Finland.
    Saccharification of lignocellulosic biomasses via ionic liquid pretreatment2016Ingår i: Industrial crops and products (Print), ISSN 0926-6690, E-ISSN 1872-633X, Vol. 92, s. 336-341Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    The current work focuses on the pretreatment efficiency of ILs combined with heat for woody biomass consisting of spruce, birch and pine as well as winter wheat straw. The latter was investigated as a comparison and with the aim to enhance its digestibility during enzymatic hydrolysis whereby the influence of IL-treatment to cellulose resistance for hydrolysis was investigated. Considering the wood species, the most common and industrially important wood species in Northern Europe were chosen in the present work and the goal was to obtain fermentable sugars and their degradation product, i.e. 5-hydroxymethylfurfural (5-HMF), which is known valuable platform chemical. Further, the differences in the yields of IL-obtainable carbohydrates between these species were studied. The highest sugar yields were obtained to glucose in the case of spruce and arabinose in the case of pine sapwood, 12.07 and 7.72 mmol/L, respectively. The highest 5-HMF yield was obtained for spruce heartwood (9.18 mmol/L) with longer treatment time, such as 100h. However, regarding woody biomass, the present work was focused more on the study and analysis of the IL-containing liquid part, wood hydrolysate, after IL-treatment aiming to answer the analysis challenges related to this fraction.

  • 12.
    Ajaikumar, Samikannu
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Ahlkvist, Johan
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Larsson, William
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Boström, Dan
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för tillämpad fysik och elektronik, Energiteknik och termisk processkemi.
    Kordas, K
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Highly active and selective bimetallic catalysts supported on transition metal oxides for the oxidation of α-pinene using molecular oxygen2010Konferensbidrag (Övrigt vetenskapligt)
  • 13.
    Ajaikumar, Samikannu
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Ahlkvist, Johan
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Larsson, William
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Boström, Dan
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för tillämpad fysik och elektronik.
    Kordas, K
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Synthesis and characterization of Cu and Cu-M (M=Co, Ni, Au and Zn) bimetallic catalysts supported on TiO2 modified SBA-152010Konferensbidrag (Övrigt vetenskapligt)
  • 14.
    Ajaikumar, Samikannu
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Ahlkvist, Johan
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Larsson, William
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Shchukarev, Andrey
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Kordas, K
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University, Piispankatu 8, FIN-20500, Turku/Åbo, Finland.
    Oxidation of α-pinene over gold containing bimetallic nanoparticles supported on reducible TiO2 by DPU method2011Ingår i: Applied Catalysis A: General, ISSN 0926-860X, E-ISSN 1873-3875, Vol. 392, nr 1-2, s. 11-18Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    A series of bimetallic catalysts Au–M (where M = Cu, Co and Ru) were supported on a reducible TiO2 oxide via deposition-precipitation (DP) method with a slow decomposition of urea as the precipitating agent. The characteristic structural features of the prepared materials were characterized by various physico-chemical techniques such as X-ray photoelectron spectroscopy (XPS), and transmission electron microscopy (TEM). XPS results indicated the formation of alloyed bimetallic particles on the TiO2 support. TEM results confirmed the fine dispersion of metal nanoparticles on the support with an average particle size in the range of 3–5 nm. An industrially important process, oxy-functionalization of α-pinene was carried out over the prepared bimetallic heterogeneous catalysts under liquid phase conditions. Reaction parameters such as the reaction time, temperature, and the effect of solvent were studied for optimal conversion of α-pinene into verbenone. The major products obtained were verbenone, verbenol, α-pinene oxide and alkyl-pinene peroxide. The activity of the catalysts followed the order; AuCu/TiO2 > AuCo/TiO2 > Cu/TiO2 > Au/TiO2 > AuRu/TiO2. Upon comparison of the various catalysts, AuCu/TiO2 was found to be an active and selective catalyst towards the formation of verbenone. The temperature, nature of the catalysts and the choice of solvents greatly influenced the reaction rate.

  • 15.
    Ajaikumar, Samikannu
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Department of Chemistry, Anna University, Guindy, Chennai, India.
    Backiaraj, Muthaiah
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University, Turku/Åbo, Finland.
    Pandurangan, Arumugam
    Transesterification of diethyl malonate with n-butanol over HPWA/MCM-41 molecular sieves2013Ingår i: Journal of porous materials, ISSN 1380-2224, E-ISSN 1573-4854, Vol. 20, nr 4, s. 951-959Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Mesoporous Si-MCM-41 and Al-MCM-41 (Si/Al = 100) materials were synthesized via a hydrothermal method. Three different ratios (10, 20 and 30 wt%) of heteropoly tungstic acid (HPWA) was loaded on Si-MCM-41 by wet impregnation techniques. The characteristic structural features of the prepared materials were studied by various physico-chemical techniques such as X-ray diffraction (XRD), Nitrogen physisorption (BET), temperature programmed desorption of ammonia (TPD) and transmission electron microscopy (TEM). Transesterification of diethyl malonate (DEM) with n-butanol under autogeneous conditions in a temperature range from 50 to 125 °C was selected as the test reaction for the as synthesized materials. The reactants were fed with various mole ratios in order to determine the optimal feed composition leading to maximum yields of transesterified products. The results indicated that the conversion of diethylmalonate depends on the HPWA concentration on the support, temperature, reaction time and mole ratio of the reactants. Further, the catalytic efficiency of HPWA/MCM-41 was compared with that of Al-MCM-41. The solid acid HPWA/MCM-41 catalysts have several advantages in comparison to conventional mineral acid catalysts which are heterogeneous, eco-friendly, highly active and selective in the formation of transesters.

  • 16. Aldea, Steliana
    et al.
    Snåre, Mathias
    Eränen, Kari
    Grenman, Henrik
    Rautio, Anne-Riika
    Kordás, Krisztian
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Johan Gadolin Process Chemistry Centre, Åbo Akademi University, Biskopsgatan 8, 20500 Åbo-Turku, Finland.
    Salmi, Tapio
    Murzin, Dmitry Y.
    Crystallization of Nano-Calcium Carbonate: The Influence of Process Parameters2016Ingår i: Chemie Ingenieur Technik, ISSN 0009-286X, E-ISSN 1522-2640, Vol. 88, nr 11, s. 1609-1616Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Precipitated calcium carbonate was synthesized by carbonation of calcium hydroxide in the presence and absence of ultrasound (conventional stirring) at atmospheric as well as at elevated pressures and different initial concentrations of Ca(OH)2. Spherical morphology of the formed calcite was favored at high Ca(OH)2 concentrations and low CO2 pressures. The presence of ultrasound did not show any influence on the reaction rate in case of efficient mixing. A small increase of the reaction rate was observed at lower CO2 pressures. Elevated pressures in combination with ultrasound did not lead to notable changes of reaction rate or particle morphology.

  • 17.
    Anugwom, I.
    et al.
    Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University, Åbo-Turku, Finland.
    Mäki-Arvela, P.
    Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University, Åbo-Turku, Finland.
    Eta, V.
    Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University, Åbo-Turku, Finland.
    Virtanen, P.
    Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University, Åbo-Turku, Finland.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University, Åbo-Turku, Finland.
    Towards optimal treatment procedure upon fractionation of Nordic lignocelluloses using novel alkanol amine – superbase ionic liquid system2012Ingår i: NWBC 2012: 4th Nordic Wood Biorefinery Conference, VTT , 2012, s. 320-322Konferensbidrag (Refereegranskat)
  • 18. Anugwom, I
    et al.
    Mäki-Arvela, P
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Extraction of nitrogen and sulphur-compounds from heavy fuel oil by 1-ethyl-3-methyl-imidazolium chloride2010Konferensbidrag (Övrigt vetenskapligt)
  • 19. Anugwom, I
    et al.
    Mäki-Arvela, P
    Salmi, T
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University, Turku, Finland.
    Ionic liquid assisted extraction of nitrogen and sulphur-containing air pollutants from model oil and regeneration of the spent ionic liquid2011Ingår i: Journal of Environmental Protection, ISSN 2152-2197, E-ISSN 2152-2219, Vol. 2, nr 6, s. 796-802Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Removal of air pollutants, such as nitrogen and sulphur containing compounds from a model oil (dodecane) was studied. An ionic liquid (1-ethyl-3-methylimidazolium chloride [C2mim] [Cl]) was used as an extractant. Liquid-liquid extraction by using 1-ethyl-3-methylimidazolium chloride [C2mim] [Cl] was found to be a very promising method for the removal of N- and S-compounds. This was evaluated by using a model oil (dodecane) with indole as a neutral nitrogen compound and pyridine as a basic nitrogen compound. Dibenzothiophene (DBT) was used as a sulphur compound. An extraction capacity of up to 90 wt% was achieved for the model oil containing pyridine, while only 76 wt% of indole in the oil was extracted. The extraction capacity of a model sulphur compound DBT was found to be up to 99 wt%. Regeneration of the spent ionic liquid was carried out with toluene back-extraction. A 1:1 toluene-to-IL wt ratio was performed at room temperature. It was observed that, for the spent ionic liquid containing DBT as a model compound more than 85 wt% (corresponding 3852 mg/kg) could be removed from the oil. After the second regeneration cycle, 86 wt% of the DBT was recovered from the ionic liquid to toluene. In the case of indole as the nitrogen containing species, more than 99 wt%, (corresponding to 2993 mg/kg) of the original indole was transferred from the model oil to the ionic liquid. After the first-regeneration cycle of the spent ionic liquid, 54 wt% of the indole–in-IL was transferred to toluene. Thus, both extractions of nitrogen and sulphur model compounds were successfully carried out from model oil and the back-extraction of these compounds from the ionic liquids to toluene demonstrated the proved the concept of the regeneration point of view.

  • 20. Anugwom, I
    et al.
    Mäki-Arvela, P
    Virtanen, P
    Willför, S
    Sjöholm, R
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Selective Extraction of Hemicelluloses from Spruce using Switchable Ionic Liquids2012Ingår i: Carbohydrate Polymers, ISSN 0144-8617, E-ISSN 1879-1344, Vol. 87, nr 3, s. 2005-2011Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Switchable Ionic Liquids (SILs) made from alcohols, either hexanol or butanol, and CO2 together with an amidine (1,8-diazabicyclo-[5.4.0]-undec-7-ene (DBU)) were investigated as dissolution/fractionation solvents for wood material. Both native spruce (Picea abies), and pre-extracted spruce were treated with either butanol SIL (SIL1) or hexanol SIL (SIL 2) for 5 days at 55 °C under normal pressure. The SILs were formed by bubbling CO2 through an equimolar mixture of either 1-hexanol or 1-butanol and DBU. The viscosity of the mixture increased from 7.1 mPas to 2980 mPas for SIL 2 and 5.1 to 1600 mPas for SIL 1. Melting points of the SILs 1 and 2 were at 8 and 14 °C, respectively. After the treatment time (5 days), the undissolved fraction contained 38 wt % less hemicelluloses compared to native spruce. There was an increase in the glucose content of the milled spruce treated with both SILs, since the milling step reduced the cellulose crystallinity of the wood and facilitated an easier SIL access into the wood. The solvents were very neutral in terms of lignin removal. Consequently, only about 2% of the lignin was removed from native wood. Moreover, a priori removal of the wood extractives did not influence the lignin removal.

    Highlights► Switchable Ionic Liquids made from, either hexanol or butanol, and CO2 together with an amidine (DBU) were studies as dissolution/fractionation solvents for spruce wood. ► After the treatment undissolved fraction contained 38 wt-% less hemicelluloses. ► We conclude that Switchable ionic liquids are effective solvent for fractionation of wood material, and they are easily recycled and can be reused.

  • 21. Anugwom, Ikenna
    et al.
    Eta, Valeri
    Mäki-Arvela, Päivi
    Virtanen, Pasi
    Lahtinen, Manu
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Process Chemistry Centre, Laboratory of Industrial Chemistry and Reaction Engineering, Åbo Akademi University, Åbo-Turku, FI-20500, Finland.
    The effect of switchable ionic liquid (SIL) treatment on the composition and crystallinity of birch chips (Betula pendula) using a novel alkanol amine-organic superbase-derived SIL2014Ingår i: Green Processing and Synthesis, ISSN 2191-9542, E-ISSN 2191-9550, Vol. 3, nr 2, s. 147-154Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Two-step treatment of birch chips (Betula pendula) was tested using diethanolamine (DEA)-1,8-diazabicyclo-[5.4.0]-undec-7-ene (DBU)-CO2-switchable ionic liquid (SIL), resulting in a 23% weight reduction in 24 h. The weight of the chips was reduced to 32% of their initial weight upon the second treatment with fresh SIL. SIL to wood ratio of 5:1, at 100°C for 24 h, without stirring, was applied in both steps. The relative amount of wood lignin reduced from 24% to 14% after two treatment cycles. The relative amount of cellulose of the undissolved fraction after SIL treatment increased from 43% (native birch wood) to 68% after the second cycle. Also, the undissolved material was efficiently fibrillated. The dissolved materials recovered from spent SIL, after treatment, contained high xylan content, about 90% of the total hemicelluloses, which was 85% of the recovered material. The powder X-ray diffraction (XRD) results revealed that the crystallinity of the undissolved material increased slightly, indicating dissolution of the amorphous material. Moreover, transformation of cellulose form I to form II in the remaining undissolved chips was not observed.

  • 22. Anugwom, Ikenna
    et al.
    Eta, Valerie
    Virtanen, Pasi
    Mäki-Arvela, Paivi
    Hedenström, Mattias
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Yibo, Ma
    Hummel, Micheal
    Sixta, Herbert
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University.
    Towards optimal selective fractionation for Nordic woody biomass using novel amine–organic superbase derived switchable ionic liquids (SILs)2014Ingår i: Biomass and Bioenergy, ISSN 0961-9534, E-ISSN 1873-2909, Vol. 70, s. 373-381Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Abstract Improved fractionation process conditions for wood dissolution with switchable ionic liquids (SILs) were determined. The short time, high temperature (STHT) system was introduced as a selective and efficient way to extract components from lignocellulosic material. A SIL based on monoethanol amine (MEA) and 1,8-diazabicyclo-[5.4.0]-undec-7-ene (DBU) formed via coupling with SO2, was applied as a solvent in a 1:3 weight ratio with water. In essence, selective dissolution of mainly lignin was achieved by means of the aqueous SIL at 160 °C (∼6.1 bar corresponding to the vapor pressure of water) in 2 h and in a pressure vessel, for both hard- and soft-wood. About 95 wt-% of wood lignin was extracted. The dissolved components in the spent SIL were recovered by the addition of an anti-solvent whereupon over 70% of the dissolved components were recovered; the recovered fraction contained 19 wt-% hemicellulose while the rest of the material was in essence lignin. The non-dissolved, fluffy material contained ∼70 wt-% cellulose and ∼20 wt-% hemicellulose – a consistency resembling that of Kraft pulp.

  • 23. Anugwom, Ikenna
    et al.
    Eta, Valerie
    Virtanen, Pasi
    Mäki-Arvela, Päivi
    Hedenström, Mattias
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Hummel, Michael
    Sixta, Herbert
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Switchable ionic liquids as delignification solvents for lignocellulosic materials2014Ingår i: ChemSusChem, ISSN 1864-5631, E-ISSN 1864-564X, Vol. 7, nr 4, s. 1170-1176Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    The transformation of lignocellulosic materials into potentially valuable resources is compromised by their complicated structure. Consequently, new economical and feasible conversion/fractionation techniques that render value-added products are intensely investigated. Herein an unorthodox and feasible fractionation method of birch chips (B. pendula) using a switchable ionic liquid (SIL) derived from an alkanol amine (monoethanol amine, MEA) and an organic super base (1,8-diazabicyclo-[5.4.0]-undec-7-ene, DBU) with two different trigger acid gases (CO2 and SO2 ) is studied. After SIL treatment, the dissolved fractions were selectively separated by a step-wise method using an antisolvent to induce precipitation. The SIL was recycled after concentration and evaporation of anti-solvent. The composition of undissolved wood after MEA-SO2 -SIL treatment resulted in 80 wt % cellulose, 10 wt % hemicelluloses, and 3 wt % lignin, whereas MEA-CO2 -SIL treatment resulted in 66 wt % cellulose, 12 wt % hemicelluloses and 11 wt % lignin. Thus, the MEA-SO2 -SIL proved more efficient than the MEA-CO2 -SIL, and a better solvent for lignin removal. All fractions were analyzed by gas chromatography (GC), Fourier transform infrared spectroscopy (FT-IR), (13) C nuclear magnetic resonance spectroscopy (NMR) and Gel permeation chromatography (GPC).

  • 24. Anugwom, Ikenna
    et al.
    Maki-Arvela, Paivi
    Virtanen, Pasi
    Willfor, Stefan
    Damlin, Pia
    Hedenström, Mattias
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Treating birch wood with a switchable 1,8-diazabicyclo-[5.4.0]-undec-7-ene-glycerol carbonate ionic liquid2012Ingår i: Holzforschung, ISSN 0018-3830, E-ISSN 1437-434X, Vol. 66, nr 7, s. 809-815Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    The suitability of a new switchable ionic liquid (SIL) has been investigated as a solvent for fractionation of lignocellulosic materials. SIL was prepared from inexpensive chemicals, e. g., glycerol, CO2, and 1,8-diazabicyclo-[5.4.0]-undec-7-ene (DBU). Fresh Nordic birch wood (B. pendula) was treated with the SIL for a time period of 1-5 days at 100 degrees C and under atmospheric pressure. Upon SIL treatment, at best, 57 % of the hemicelluloses were dissolved and 50 % of lignins were dissolved from the native birch. The slightly fibrillated SIL treated chips contained about 55 % cellulose. Up to 76 % of the recovered species removed from the spent SIL liquor was originating from hemicelluloses, mainly from xylan. The spent SILs were reused for fresh wood dissolution in four consecutive cycles and each time the wood dissolution efficiency was similar. SILs could offer affordable (easy-to-synthesize) solvent systems for partial elimination of hemicelluloses and lignin from wood. SILs can also be prepared in-situ and on-site.

  • 25. Anugwom, Ikenna
    et al.
    Mäki-Arvela, Päivi
    Virtanen, Pasi
    Damlin, Pia
    Sjöholm, Rainer
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Switchable ionic liquids (SILs) based on glycerol and acid gases 2011Ingår i: RSC Advances, ISSN 2046-2069, Vol. 1, nr 3, s. 452-457Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    New types of switchable ionic liquids (SILs), containing 1,8-diazabicyclo-[5.4.0]-undec-7-ene (DBU), glycerol and an acid gas (CO2, SO2), were synthesized and characterized in this study. [DBU][Carbonate] or [sulfonate] were easily synthesized from a non-ionic mixture of molecular organic polyol and amidine base upon bubbling of an acid gas (CO2, SO2). Moreover, they were switched back to the original molecular solvents by flushing out the acid gas (CO2, SO2) by heating and/or bubbling an inert gas such as N2 through it. The structures of the SILs were confirmed by NMR and FTIR. The change from low polarity (molecular solvent) to high polarity (Switchable Ionic Liquid, SIL) was also indicated by the changes in properties, such as viscosity and miscibility with different organic solvents. The decomposition temperatures of the SILs were determined by means of Thermo Gravimetric Analysis (TGA) and gave values in the range of 50 °C and 120 °C for DBU-glycerol-CO2 (SIL1) and DBU-glycerol-SO2 (SIL2), respectively. Due to the reasonable decomposition temperatures, these novel SILs can be employed in multiple applications.

  • 26.
    Anugwom, Ikenna
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University, Åbo-Turku FI-20500, Finland.
    Rujana, L.
    Wärnå, J.
    Hedenström, Mattias
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University, Åbo-Turku FI-20500, Finland.
    In quest for the optimal delignification of lignocellulosic biomass using hydrated, SO2 switched DBU MEASIL switchable ionic liquid2016Ingår i: Chemical Engineering Journal, ISSN 1385-8947, E-ISSN 1873-3212, Vol. 297, s. 256-264Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    In this paper, various process parameters aiming at optimal short-time-high-temperature (STHT) process were studied upon fractionation of Nordic woody biomass into its primary constituents. Highly diluted, aqueous 'SO2-switched' switchable ionic liquid (SIL) based on an alkanol amine (monoethanol amine, MEA) and an organic superbase (1,8-diazabicyclo-[5.4.0]-undec-7-ene, DBU) was applied. The ultimate goal was to develop a more sustainable, environmentally friendly and cost efficient systems for efficient separation of the lignocellulosic fractions. One of the main products from the SIL fractionation is cellulose-rich pulp with very low lignin content, complemented with hemicelluloses. The NMR results reveal that substantial removal of lignin occurs even when relatively low amount of SIL was used. Further, a simple mathematical model describing the dissolution of the lignocellulose components (hemicellulose and lignin) and weight loss of wood as a function of time is described. Moreover, the most efficient process involved the use of SpinChem (R) rotating bed reactor while upon use of a flow through (loop) reactor, promising results were obtained at a treatment time of 4 h. Still, all the reactor systems studied gave rise to a rather low removal of hemicelluloses which mean that the solvent system is primary selective towards lignin dissolution.

  • 27. Asres, Georgies Alene
    et al.
    Baldoví, José J.
    Dombovari, Aron
    Järvinen, Topias
    Lorite, Gabriela Simone
    Mohl, Melinda
    Shchukarev, Andrey
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Pérez Paz, Alejandro
    Xian, Lede
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Industrial Chemistry & Reaction Engineering, Department of Chemical Engineering, Johan Gadolin Process Chemistry Centre, Åbo Akademi University, Åbo-Turku, Finland.
    Spetz, Anita Lloyd
    Jantunen, Heli
    Rubio, Ángel
    Kordás, Krisztian
    Ultrasensitive H2S gas sensors based on p-type WS2 hybrid materials2018Ingår i: Nano Reseach, ISSN 1998-0124, E-ISSN 1998-0000, Vol. 11, nr 8, s. 4215-4224Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Owing to their higher intrinsic electrical conductivity and chemical stability with respect to their oxide counterparts, nanostructured metal sulfides are expected to revive materials for resistive chemical sensor applications. Herein, we explore the gas sensing behavior of WS2 nanowire-nanoflake hybrid materials and demonstrate their excellent sensitivity (0.043 ppm-1) as well as high selectivity towards H2S relative to CO, NH3, H2, and NO (with corresponding sensitivities of 0.002, 0.0074, 0.0002, and 0.0046 ppm-1, respectively). Gas response measurements, complemented with the results of X-ray photoelectron spectroscopy analysis and first-principles calculations based on density functional theory, suggest that the intrinsic electronic properties of pristine WS2 alone are not sufficient to explain the observed high sensitivity towards H2S. A major role in this behavior is also played by O doping in the S sites of the WS2 lattice. The results of the present study open up new avenues for the use of transition metal disulfide nanomaterials as effective alternatives to metal oxides in future applications for industrial process control, security, and health and environmental safety.

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  • 28. Bawuaha, Prince
    et al.
    Silfsten, Pertti
    Sarkar, Anjana
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Kordas, Kristian
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Peiponen, Kai-Erik
    On the complex refractive index of N-doped TiO2 nanospheres and nanowires in the terahertz spectral region2013Ingår i: Vibrational Spectroscopy, ISSN 0924-2031, E-ISSN 1873-3697, Vol. 68, s. 241-245Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    In this paper, the terahertz (THz) transmission measurement technique was applied to characterize titanium dioxide (TiO2) nanospheres and nanowires subjected to thermal treatments under various conditions. Differences in the spectral features of the nanospheres and nanowires were observed due to treatment and annealing of the samples in different gas atmospheres. The observations made can be explained based on the formation of new phonon bands and/or widening of the phonon bands due to polymorphism. A singly subtractive Kramers Kronig dispersion relation was utilized to estimate the frequency-dependent real refractive index of the various samples, having a priori unknown sample thickness, from the absorbance data.

  • 29. Behravesh, Erfan
    et al.
    Kumar, Narendra
    Balme, Quentin
    Roine, Jorma
    Salonen, Jarno
    Shchukarev, Andrey
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Process Chemistry Centre, Åbo Akademi University, FI-20500 Turku/Åbo, Finland.
    Peurla, Markus
    Aho, Atte
    Eränen, Kari
    Murzin, Dmitry Yu.
    Salmi, Tapio
    Synthesis and characterization of Au nano particles supported catalysts for partial oxidation of ethanol: Influence of solution pH, Au nanoparticle size, support structure and acidity2017Ingår i: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 353, s. 223-238Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Partial oxidation of ethanol to acetaldehyde was carried out over gold catalysts supported on various oxides and zeolites by deposition precipitation. The special focus of this work was on the influence of H-Y zeolite surface charge on Au cluster size and loading linking it to activity and selectivity in ethanol oxidation and comparing with other studied catalysts. The catalysts were characterized by nitrogen physisorption, transmission electron microscopy (TEM), scanning electron microscopy/energy dispersive X-ray analysis (SEM/EDXA), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FTIR) and zeta potential measurements. pH of the solution governed the Au NPs size within the range of 5.8–13.2 nm with less negatively charged surfaces leading to formation of smaller clusters. Au loading on H-Y zeolite with silica to alumina ratio of 80 was increased by raising the pH. In fact, H-Y-12 and H-Beta-25 were selective towards diethyl ether while acetaldehyde was the prevalent product on less acidic H-Y-80. The results demonstrated strong dependency of the catalytic activity on the Au cluster size. Namely turn over frequency (TOF) decreased with an increase in metal size from 6.3 to 9.3 nm on H-Y-80. Selectivity towards acetaldehyde and ethyl acetate did not change significantly on H-Y-80 within 6.3–9.3 nm Au particle size range. On Al2O3 support, however, selectivity towards acetaldehyde increased considerably upon diminishing Au average particle size from 3.7 to 2.1 nm.

  • 30. Berglund, Linn
    et al.
    Anugwom, Ikenna
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Johan Gadolin Process Chemistry Centre, Åbo Akademi University, Turku, Finland.
    Hedenström, Mattias
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Aitomäki, Yvonne
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Johan Gadolin Process Chemistry Centre, Åbo Akademi University, Turku, Finland.
    Oksman, Kristiina
    Switchable ionic liquids enable efficient nanofibrillation of wood pulp2017Ingår i: Cellulose, ISSN 0969-0239, E-ISSN 1572-882X, Vol. 24, nr 8, s. 3265-3279Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Use of switchable ionic liquid (SIL) pulp offers an efficient and greener technology to produce nanofibers via ultrafine grinding. In this study, we demonstrate that SIL pulp opens up a mechanically efficient route to the nanofibrillation of wood pulp, thus providing both a low cost and chemically benign route to the production of cellulose nanofibers. The degree of fibrillation during the process was evaluated by viscosity and optical microscopy of SIL treated, bleached SIL treated and a reference pulp. Furthermore, films were prepared from the fibrillated material for characterization and tensile testing. It was observed that substantially improved mechanical properties were attained as a result of the grinding process, thus signifying nanofibrillation. Both SIL treated and bleached SIL treated pulps were fibrillated into nanofibers with fiber diameters below 15 nm thus forming networks of hydrophilic nature with an intact crystalline structure. Notably, it was found that the SIL pulp could be fibrillated more efficiently than traditional pulp since nanofibers could be produced with more than 30% less energy when compared to the reference pulp. Additionally, bleaching reduced the energy demand by further 16%. The study demonstrated that this switchable ionic liquid treatment has considerable potential in the commercial production of nanofibers due to the increased efficiency in fibrillation.

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  • 31.
    Bernardini, A.
    et al.
    Padova, Italy.
    Gemo, N.
    Turku/Åbo, Finland; .
    Biasi, Paolo
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Canu, P.
    Padova, Italy.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Salmi, T.
    Turku/Åbo, Finland; .
    Lanza, R.
    Stockholm, Sweden.
    Direct synthesis of H2O2 over Pd supported on rare earths promoted zirconia2015Ingår i: Catalysis Today, ISSN 0920-5861, E-ISSN 1873-4308, Vol. 256, nr 2, s. 294-301Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    In this work Pd (0.3 or 0.6 wt.%) was supported on both ZrxM1-xO2 (M = La, Y, Ce) and on mechanical mixtures of CeO2 and ZrO2. The synthesized catalysts were characterized by XRD, TPR, AAS and CO chemisorption and tested for the direct synthesis of hydrogen peroxide in a high pressure semibatch apparatus. The reactants conversion was limited in order to avoid mass-transfer limitations. No selectivity enhancers of any kind were used and the all the materials were halide free. Small metal particles were obtained (1-2.6 nm). Supports with smaller pore diameters leaded to larger Pd particles, which in turn were found to preferentially support the formation of the peroxide. Moreover, supports with higher reducibility favored the production of H2O2, probably due to an easier reduction of the active metal, essential to achieve high selectivity. Notwithstanding the absence of enhancers, the specific activity and selectivity recorded were very high. (C) 2015 Elsevier B.V. All rights reserved.

  • 32. Bernas, Andreas
    et al.
    Salmi, Tapio
    Murzin, Dmitry Yu
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Rintola, Mikko
    Catalytic transformation of abietic acid to hydrocarbons2012Ingår i: Topics in catalysis, ISSN 1022-5528, E-ISSN 1572-9028, Vol. 55, nr 7-10, s. 673-679Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Catalytic and thermal conversion of abietic acid was investigated in a laboratory scale high-pressure autoclave. Fractionation of crude tall oil produces rosin acids of which abietic acid is the main compound. Tall oil rosin acid, a forest product industry residue, is an abundant, inexpensive and chemically desirable feedstock for production of lighter hydrocarbons that can be used as diesel fuel additives. The carboxylic acid functionality of the main reactant, abietic acid, must first be removed, followed by double bond hydrogenation of the remaining aromatic rings. In this study, a number of catalytic and non-catalytic reaction steps in the conversion of abietic acid were investigated. The aim was to study hydrogenation and decarboxylation reactions of abietic acid in order to produce lighter hydrocarbons. The experiments were performed by using toluene as a solvent as well as with neat abietic acid, in the absence of any solvent. Hydrogenation of abietic acid to tetrahydroabietic acid in toluene was successfully performed over palladium on carbon catalyst at the temperature range of 100-200 A degrees C and at 30 bar hydrogen pressure. Thermal non-catalytic decarboxylation of abietic acid in toluene takes place at 200-300 A degrees C resulting in one main product. The hydrocarbon products were further hydrogenated under hydrogen pressure. Catalytic decarboxylation of abietic acid in toluene was achieved over 5 wt% Ru/C, giving a wider product distribution than thermal decarboxylation.

  • 33.
    Biasi, P.
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Åbo Akad Univ, Dept Chem Engn, Lab Ind Chem & React Engn, Johan Gadolin Proc Chem Ctr PCC, Biskopsgatan 8, FI-20500 Turku, Finland.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Åbo Akad Univ, Dept Chem Engn, Lab Ind Chem & React Engn, Johan Gadolin Proc Chem Ctr PCC, Biskopsgatan 8, FI-20500 Turku, Finland.
    Sterchele, S.
    Salmi, T.
    Gemo, N.
    Shchukarev, Andrey
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Centomo, P.
    Zecca, M.
    Canu, P.
    Rautio, A. -R
    Kordàs, K.
    Revealing the role of bromide in the H2O2 direct synthesis with the catalyst wet pretreatment method (CWPM)2017Ingår i: AIChE Journal, ISSN 0001-1541, E-ISSN 1547-5905, Vol. 63, nr 1, s. 32-42Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    A tailor-made Pd0/K2621 catalyst was subjected to post synthesis modification via a wet treatment procedure. The aimwas the understanding of the role of promoters and how—if any—improvements could be qualitatively related to the cat-alyst performance for the H2O2direct synthesis. The Catalyst Wet Pretreatment Method was applied in different metha-nolic solutions containing H2O2, NaBr, and H3PO4, either as single modifiers or as a mixture. The catalyst wascharacterized by Transmission Electron Microscopy and X-ray Photoelectron Spectroscopy. It was concluded that themodified catalysts give rise to higher selectivities compared to the pristi ne reference catalyst thus opening a possibilityto exclude the addit ion of the undesirable selectivity enhancers in the reaction medium. This work provides original evi-dence on the role of promoter s, especially bromide, allowing the formulation of a new reaction mechanism for one ofthe most challenging reactions recognized by the world.

  • 34.
    Biasi, P.
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Department of Chemical Engineering, Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre (PCC), Åbo Akademi University, Åbo-Turku, Finland.
    Salmi, T.
    Department of Chemical Engineering, Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre (PCC), Åbo Akademi University, Åbo-Turku, Finland.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Department of Chemical Engineering, Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre (PCC), Åbo Akademi University, Åbo-Turku, Finland.
    Tailoring the process of H2O2 direct synthesis: Catalyst design and reaction engineering to reach an industrial feasibility2014Ingår i: 21st International Congress of Chemical and Process Engineering, CHISA 2014 and 17th Conference on Process Integration, Modelling and Optimisation for Energy Saving and Pollution Reduction, PRES 2014, Czech Society of Chemical Engineering , 2014, s. 65-65Konferensbidrag (Refereegranskat)
  • 35. Biasi, Pierdomenico
    et al.
    Serna, Juan Garcia
    Salmi, Tapio O.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Department of Chemical Engineering, Process Chemistry Centre (PCC), Laboratory of Industrial Chemistry and Reaction Engineering, Åbo Akademi University, ÅBO-TURKU, Finland.
    Hydrogen Peroxide Direct Synthesis: Enhancement of Selectivity and Production with non-Conventional Methods2013Ingår i: ICHEAP-11: 11TH INTERNATIONAL CONFERENCE ON CHEMICAL AND PROCESS ENGINEERING, PTS 1-4 / [ed] Pierucci, S, Klemes, JJ, AIDIC - associazione italiana di ingegneria chimica, 2013, s. 673-678Konferensbidrag (Refereegranskat)
    Abstract [en]

    The present work is part of a comprehensive study on the direct synthesis of hydrogen peroxide in different fields, from chemistry to chemical engineering. Working on the different fields of the direct synthesis gave the possibility to look at the results and the challenges from different viewpoints. Here was investigated one parameter that enhances the direct synthesis. The H-2/Pd ratio is the key parameter that has to be investigated and optimize to enhance the hydrogen peroxide direct synthesis. Two reactors were built to study deeply the H-2/Pd ratio and to demonstrate how this parameter can affect the direct synthesis both in batch and continuous reactor with non-conventional experiments/methods. 1) A batch reactor was utilized as a "starving reactor" to enhance the productivity of hydrogen peroxide and to try to keep constant the selectivity. The starving method consists in refilling the hydrogen when it is consumed in the reactor. 2) A trickle bed reactor was utilized with a gradient of catalyst along the reactor to maximize both production and selectivity of hydrogen peroxide. The distribution of the catalyst along the bed gave the possibility to significantly improve the selectivity and the production of hydrogen peroxide (up to 0.5% in selected conditions). Higher production rate and selectivity were found when the catalyst concentration decreases along the bed from the top to the bottom compared to the uniformly dispersed catalyst. Selectivity in the batch reactor was enhanced by 5% and in the continuous reactor of 10%. The non-conventional experimental methods have been found to be novelty concepts to enhance the hydrogen peroxide direct synthesis.

  • 36.
    Biasi, Pierdomenico
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Industrial Chemistry and Reaction Engineering, Process Chemistry Center (PCC), Department of Chemical Engineering, Åbo Akademi University,Turku/Åbo, Finland.
    Sterchele, Stefano
    Bizzotto, Francesco
    Manzoli, Maela
    Lindholm, Sten
    Ek, Paul
    Bobacka, Johan
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Industrial Chemistry and Reaction Engineering, Process Chemistry Center (PCC), Department of Chemical Engineering, Åbo Akademi University,Turku/Åbo, Finland.
    Salmi, Tapio
    Application of the Catalyst Wet Pretreatment Method (CWPM) for catalytic direct synthesis of H2O22015Ingår i: Catalysis Today, ISSN 0920-5861, E-ISSN 1873-4308, Vol. 246, nr Special Issue, s. 207-215Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    This work concerns a new technique to post-modify the catalytic material intended for use in H2O2 direct synthesis. The catalyst chosen was a commercially available 1 wt.% Pd/C. The catalyst was modified with the so-called Catalyst Wet Pretreatment Method (CWPM) that is used to post-modify prepared catalysts with aqueous solutions of NaBr, in different concentrations. The performance of pristine and the pretreated materials were then compared in the H2O2 direct synthesis and characterized before and after the catalytic tests in order to understand the role of the different concentrations of bromide in the CWPM procedure. The surface features of the different catalysts were analyzed with CO chemisorption (metal dispersion and mean particle size), Transmission Electron Microscopy (TEM, for Pd morphology and Pd particle size distributions), Inductive Coupled Plasma (ICP, for Pd content) and Ion Chromatography (IC, for bromide content). Various features of the materials prepared with the CWPM were correlated with the catalytic performance. It was found that the bromide has an active role in the reconstruction of metal phase and it does not only act as a poison for the most active catalytic sites as often reported in literature. By using this new protocol, the production H2O2 was almost doubled compared to the non-modified material when no direct promoters were added to the reaction environment.

  • 37. Borah, Raju Kumar
    et al.
    Raul, Prasanta Kumar
    Mahanta, Abhijit
    Shchukarev, Andrey
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Industrial Chemistry & Reaction Engineering, Åbo Akademi University, Åbo-Turku, Finland.
    Thakur, Ashim Jyoti
    Copper Oxide Nanoparticles as a Mild and Efficient Catalyst for N-Arylation of Imidazole and Aniline with Boronic Acids at Room Temperature2017Ingår i: Synlett: Accounts and Rapid Communications in Synthetic Organic Chemistry, ISSN 0936-5214, E-ISSN 1437-2096, Vol. 28, nr 10, s. 1177-1182Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    The present work describes the excellent catalytic activity of copper(II) oxide nanoparticles (NPs) towards N-arylation of aniline and imidazole at room temperature. The copper(II) oxide NPs were synthesized by a thermal refluxing technique and characterized by FT-IR spectroscopy; powder XRD, SEM, EDX, TEM, TGA, XPS, BET surface area analysis, and particle size analysis. The size of the NPs was found to be around 12 nm having a surface area of 164.180 m(2) g(-1). The catalytic system was also found to be recyclable and could be reused in subsequent catalytic runs without a significant loss of activity.

  • 38.
    Bourajoini, Hasna
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Kordas, K.
    Microelectronics and Materials Physics Laboratories, Department of Electrical Engineering, University of Oulu, University of Oulu, Finland.
    Larsson, W.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University, Åbo-Turku, Finland.
    Synthesis of calcium manganese oxides - Unravelling the natures secrets2014Ingår i: 21st International Congress of Chemical and Process Engineering, CHISA 2014 and 17th Conference on Process Integration, Modelling and Optimisation for Energy Saving and Pollution Reduction, PRES 2014, Czech Society of Chemical Engineering , 2014, s. 371-371, artikel-id P3.95Konferensbidrag (Refereegranskat)
  • 39.
    Bourajoini, Hasna
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Rautio, Anne-Riikka
    Kordas, Krisztian
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Calcium manganese oxide catalysts for water oxidation: Unravelling the influence of various synthesis strategies2016Ingår i: Materials research bulletin, ISSN 0025-5408, E-ISSN 1873-4227, Vol. 79, s. 133-137Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Abstract Three different mixed oxide catalysts primarily consisting of calcium and manganese oxides targeting artificial photosynthesis were synthesized and studied. According to the results, their catalytic activity for water oxidation was enhanced by the presence of mixed valence states of Mnn+ ions (3.0 ≤ n ≪ 4.0), while the specific surface area had negligible effect.

  • 40.
    Bui, Thai Q.
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Khokarale, Santosh G.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Shukla, Shashi Kant
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Switchable aqueous pentaethylenehexamine for CO2 capture and beyond2018Ingår i: 23rd International Congress of Chemical and Process Engineering, CHISA 2018 and 21st Conference on Process Integration, Modelling and Optimisation for Energy Saving and Pollution Reduction, PRES 2018, Czech Society of Chemical Engineering , 2018, s. 143-144Konferensbidrag (Refereegranskat)
  • 41.
    Bui, Thai Q.
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Khokarale, Santosh G.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Shukla, Shashi Kant
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Industrial Chemistry & Reaction Engineering, Department of Chemical Engineering, Johan Gadolin Process Chemistry Centre, Åbo Akademi University, Biskopsgatan 8, FI-20500 Åbo-Turku, Finland.
    Switchable Aqueous Pentaethylenehexamine System for CO2 Capture: an Alternative Technology with Industrial Potential2018Ingår i: ACS Sustainable Chemistry and Engineering, E-ISSN 2168-0485, Vol. 6, nr 8, s. 10395-10407Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Herein we report the application of polyamine pentaethylenehexamine (PEHA, 3,6,9,12-tetraazatetradecane-1,14-diamine) in CO2 absorption with both neat PEHA and aqueous solutions thereof. The absorption of molecular CO2 in pure PEHA and in PEHA-water systems resulted in the formation of two chemical species, namely, PEHA carbamate and bicarbonate. It was observed that, upon formation of these species, both the CO2 absorption capacity and CO2 absorption rate were controlled by the amount of water in the system. During the CO2 absorption, the neat PEHA and 92 wt % PEHA were capable of forming carbamate species only while other aqueous analogues with higher dilution allowed for the formation of both carbamate and bicarbonate species upon exceeding 8 wt % water in the mixture. The CO2 uptake steadily increased with an increase in the water concentration in the solvent mixture and reached the maximum value of 0.25 g of CO2/(g of solvent) in the case of 56 wt % PEHA in water. However, in the case of more dilute systems (i.e., <56 wt % PEHA in water), the trend reversed and the CO2 loading decreased linearly to 0.05 g of CO2/(g of solvent) for 11 wt % PEHA in water. Meanwhile, it usually took shorter time to achieve the full CO2 absorption capacity (equilibrium) with increasing water content in all cases. The C-13 NMR analysis was used to quantify the relative amount of PEHA carbamate and bicarbonate, respectively, in reaction mixtures. The Kamle-Taft parameters (alpha, beta, and pi*) of aqueous solutions for different concentrations of PEHA were also studied taking advantage of various solvatochromic dyes and correlated with the CO2 absorption capacity. The thermally induced switchable nature of CO2-saturated neat and aqueous PEHA solutions for transformation of ionic PEHA carbamate and bicarbonate moieties to molecular PEHA is also represented. A comparison between aqueous PEHA and aqueous monoethanolamine (industrial solvent) for CO2 capture is reported. Hence, most importantly, a switchable PEHA system is demonstrated for reversible CO2 absorption processes.

  • 42.
    Bui, Thai Q.
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Konwar, Lakhya Jyoti
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Samikannu, Ajaikumar
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Nikjoo, Dariush
    Division of Materials Science, Luleå University of Technology, Luleå, Sweden.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Johan Gadolin Process Chemistry Centre, Åbo Akademi University, Turku, Finland.
    Mesoporous Melamine-Formaldehyde Resins as Efficient Heterogeneous Catalyst for Continuous Synthesis of Cyclic Carbonates from Epoxides and gaseous CO22020Ingår i: ACS Sustainable Chemistry and Engineering, E-ISSN 2168-0485, Vol. 8, nr 34, s. 12852-12869Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Herein we report the application of inexpensive mesoporous melamine-formaldehyde resins (MMFR and MMFR250) obtained by a novel template-free and organosolvent-free hydrothermal method as efficient heterogeneous catalysts for direct synthesis of cyclic carbonates from CO2 and epoxides (epichlorohydrin, butylene oxide and styrene oxide). The catalytic activity of the melamine resins was attributed to the abundant Lewis basic N-sites capable of activating CO2 molecules. Based on CO2-Temperature programmed desorption, the concentration of surface basic sites for MMFR and MMFR250 were estimated to be 172 and 56 µmol/g, while the activation energy of CO2 desorption (strength of basic sites) were calculated to be 92.1 and 64.5 kJ/mol. We also observed considerable differences in the catalytic activity and stability of polymeric catalysts in batch and in continuous-flow mode; due to the existence of a synergism between adsorption of CO2 and cyclic carbonates (poison). Our experiments also revealed important role of catalyst surface chemistry and CO2 partial pressure upon catalyst poisoning. Nevertheless, owing to their unique properties (large specific surface area, large mesoporous and CO2 basicity) melamine resins presented excellent activity (turnover frequency 207-2147 h-1), selectivity (>99%) for carbonation of epoxides with CO2 (20 bar initial CO2 or CO2:epoxide mole ratio ~1.5) under solvent-free and co-catalyst-free conditions at 100-120 oC. Most importantly, these low-cost polymeric catalysts were reusable and demonstrated exceptional stability in a flow reactor (tested upto 13 days time on stream, weight hourly space velocity 0.26-1.91 h-1) for continuous cyclic carbonate production from gaseous CO2 with different epoxides (conversion 76-100% and selectivity >99%) under industrially relevant conditions (120 oC, 13 bar, solvent-free/co-catalyst-free) confirming their superiority over the previously reported catalytic materials.

  • 43.
    Bukhanko, Natalia
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Larsson, William
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Samikannu, Ajaikumar
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University, Turku/Åbo, Finland.
    Gas phase synthesis of 'green' ethyl chloride2012Konferensbidrag (Refereegranskat)
    Abstract [en]

    Various xZnCl2/Al2O3 (x = 0-2 wt %) catalysts, and the effect of the type of alumina in the gas phase synthesis of ethyl chloride from ethyl alcohol and HCl were studied. The influence of temperature, pressure, and feed composition was investigated. The nature of catalytic material significantly influenced the performance of the system. The tailor-made high-porous Al2O3 was the optimal catalyst that showed high conversion and selectivity. At 325°C, the conversion obtained was 94-96% and selectivity remained at a constant level of 98% throughout the experiment. This is an abstract of a paper presented at the CHISA 2012 - 20th International Congress of Chemical and Process Engineering and PRES 2012 - 15th Conference PRES (Prague, Czech Republic 8/25-29/2012).

  • 44.
    Bukhanko, Natalia
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Larsson, William
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Samikannu, Ajaikumar
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Wärnå, Johan
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University, Biskopsgatan, 8, Turku/Åbo, Finland.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University, Biskopsgatan, 8, Turku/Åbo, Finland.
    Gas phase synthesis of isopropyl chloride from isopropanol and HCl over alumina catalysts2014Ingår i: 21st International Congress of Chemical and Process Engineering, CHISA 2014 and 17th Conference on Process Integration, Modelling and Optimisation for Energy Saving and Pollution Reduction, PRES 2014, Czech Society of Chemical Engineering , 2014, s. 72-73Konferensbidrag (Refereegranskat)
  • 45.
    Bukhanko, Natalia
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Samikannu, Ajaikumar
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Larsson, William
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Shchukarev, Andrey
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Leino, Anne-Riikka
    Microelectronics and Materials Physics Laboratories, University of Oulu, Finland.
    Kordas, Krisztian
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Microelectronics and Materials Physics Laboratories, University of Oulu, Finland.
    Wärnå, Johan
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University, Finland.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Process Chemistry Centre, Åbo Akademi University, Finland.
    Continuous gas phase synthesis of 1-ethyl chloride from ethyl alcohol and hydrochloric acid over Al2O3-based catalysts: the ‘green’ route2013Ingår i: ACS Sustainable Chemistry and Engineering, E-ISSN 2168-0485, Vol. 1, nr 8, s. 883-893Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    The synthesis of 1-ethyl chloride in the gas-phase mixture of ethanol and hydrochloric acid over ZnCl2/Al2O3 catalysts was studied in a continuous reactor using both commercial and tailor-made supports. The catalytic materials were characterized by the means of structural (XPS, TEM, XRD, and BET) and catalytic activity (selectivity and conversion) measurements. The reaction parameters such as temperature, pressure, and feedstock flow rates were optimized for the conversion of ethanol to ethyl chloride. The new tailor-made highly porous Al2O3-based catalyst outperformed its commercial counterpart by exhibiting high conversion and selectivity (98%) at the temperature of 325 °C. Long-term stability tests (240 h) confirmed the excellent durability of the tailor-made alumina catalysts. The process demonstrated here poses an efficient and economic “green” large-scale on-site synthesis of this industrially important reactant in industry, where bioethanol is produced and 1-ethyl chloride is necessary, e.g., for ethylation of cellulose and synthetic polymer products. On-site in situ production of ethyl chloride avoids the problems associated with the transportation and storage of toxic and flammable 1-ethyl chloride.

  • 46.
    Bukhanko, Natalia
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Department of Forest Biomaterials Technology, Swedish University of Agricultural Science, Umeå, Sweden.
    Schwarz, Christopher
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Samikannu, Ajaikumar
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Ngoc Pham, Tung
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Department of Chemistry, The University of Danang - University of Science and Technology, Nguyen Luong Bang, Lien Chieu, Da Nang, Viet Nam.
    Siljebo, William
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Wärnå, Johan
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Shchukarev, Andrey
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Rautio, Anne-Riikka
    Kordas, Krisztian
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Gas phase synthesis of isopropyl chloride from isopropanol and HCl over alumina and flexible 3-D carbon foam supported catalysts2017Ingår i: Applied Catalysis A: General, ISSN 0926-860X, E-ISSN 1873-3875, Vol. 542, nr 25, s. 212-225Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Isopropyl chloride synthesis from isopropanol and HCl in gas phase over ZnCl2 catalysts supported on Al2O3 as well as flexible carbon foam was studied in a continuous reactor. A series of catalytic materials were synthesised and characterised by BET, XPS, SEM, TEM, XRD and NH3-TPD methods. Catalytic activity tests (product selectivity and conversion of reactants) were performed for all materials and optimal reaction conditions (temperature and feedstock flow rates) were found. The results indicate that the highest yield of isopropyl chloride was obtained over 5 wt.% ZnCl2 on commercial Al2O3 (No. II) (95.3%). Determination of product mixture compositions and by-product identification were done using a GC-MS method. Carbon foam variant catalyst, 5 wt.% ZnCl2/C, was found to perform best out of the carbon-supported materials, achieving ∼75% yield of isopropyl chloride. The kinetic model describing the process in a continuous packed bed reactor was proposed and kinetic parameters were calculated. The activation energy for the formation of isopropyl chloride reaction directly from isopropanol and HCl was found to be ∼58 kJ/mol.

  • 47.
    Bukhanko, Natalia
    et al.
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Wärnå, Johan
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Johan Gadolin Process Chemistry Centre, Åbo Akademi University, Biskopsgatan 8, FIN-20500, Turku/Åbo, Finland.
    Samikannu, Ajaikumar
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Johan Gadolin Process Chemistry Centre, Åbo Akademi University, Biskopsgatan 8, FIN-20500, Turku/Åbo, Finland.
    Kinetic modeling of gas phase synthesis of ethyl chloride from ethanol and HCl in fixed bed reactor2016Ingår i: Chemical Engineering Science, ISSN 0009-2509, E-ISSN 1873-4405, Vol. 142, s. 310-317Artikel i tidskrift (Refereegranskat)
    Abstract [en]

    Kinetic modeling of gas-phase synthesis of ethyl chloride from ethanol and hydrochloric acid over high porous Al2O3 and 2 wt% ZnCl2/Al2O3 catalysts was studied in a continuous plug flow reactor in the temperature range of 200–325 °C. Two rival kinetic models were proposed that both describe the kinetics well. The kinetic parameters of the reaction were determined and activation energy values for ethyl chloride formation from ethyl alcohol and diethyl ether reactions were calculated.

  • 48.
    Conte, Ricardo Pezoa
    et al.
    Industrial Chemistry and Reaction Engineering Johan Gadolin Process Chemistry Centre, Åbo Akademi University, Åbo-Turku, Finland.
    Ravanal, M. Cristina
    Centre for Biochemical Engineering and Biotechnology, Department of Chemical Engineering and Biotechnology, University of Chile, Santiago, Chile.
    Mäki-Arvela, Päivi
    Industrial Chemistry and Reaction Engineering Johan Gadolin Process Chemistry Centre, Åbo Akademi University, Åbo-Turku, Finland.
    Willför, Stefan
    Wood and Paper Chemistry Johan Gadolin Process Chemistry Centre, Åbo Akademi University, Åbo-Turku, Finland.
    Lienqueo, M. Elena
    Centre for Biochemical Engineering and Biotechnology, Department of Chemical Engineering and Biotechnology, University of Chile, Santiago, Chile.
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Industrial Chemistry and Reaction Engineering Johan Gadolin Process Chemistry Centre, Åbo Akademi University, Åbo-Turku, Finland.
    Bioethanol production from the green alga ulva rigida and the brown algae macrocystis pyrifera2015Ingår i: NWBC 2015: the 6th Nordic Wood Biorefinery Conference, VTT Technical Research Centre of Finland , 2015, s. 319-325Konferensbidrag (Refereegranskat)
    Abstract [en]

    Macroalgae are suitable bioresources to be explored as raw material for bioethanol production, as about 40 wt.% of its mass is composed of carbohydrates and they completely lack lignin. In this work the simultaneous saccharification and fermentation (SSF) of the green alga Ulva rigida and the brown alga Macrocystis pyrifera was performed. The algae were initially pretreated in deionized water or diluted sulfuric acid at 125°C in an autoclave for 60 min, respectively. Commercial cellulolytic enzymes and yeast were used for ethanol production. The carbohydrate composition of the fresh alga, pretreated alga and glucose and ethanol concentrations in the SSF processing are given. The water pretreatment solubilized 82 wt.% of the ulvan (rhamno-glucuroxylan) contained in U. rigida and 73 wt.% of the glucan remained in the residue. The diluted acid treatment removed 93 wt.% of the carbohydrates contained in U. rigida. The SSF of U. rigida pretreated with water produced 0.47 g EtOH/g sugar, with a 92 wt.% theoretical yield. In turn, water and diluted acid pretreatment of M. pyrifera increased 8.4 and 14.8 fold the carbohydrate content in the pretreated alga compared to the SSF of the fresh alga. The SSF of M. pyrifera pretreated with dilute sulfuric acid produced 0.15 g EtOH/g sugar, 29 wt.% theoretical yield. The production of ethanol was demonstrated for U. rigida and M. pyrifera with mild pretreatments. Especially in case of U. rigida simple water treatment allows to isolate ulvan for other purposes and efficiently ferment the remaining fibers.

  • 49. Cortinez, V
    et al.
    Hyvärinen, S
    Reunanen, M
    Hemming, J
    Lienqueo, M E
    Murzin, D Yu
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Evaluation of ionic liquid mediated pretreatment for the enzymatic hydrolysis of forest residues to obtain bioethanol2009Konferensbidrag (Övrigt vetenskapligt)
  • 50. Cortinez, V
    et al.
    Hyvärinen, S
    Reunanen, M
    Hemming, J
    Murzin, D Yu
    Mikkola, Jyri-Pekka
    Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
    Lienqueo, ME
     Pretreatment with ionic líquids of Lenga (Nothofagus pumilio) and Eucalyptus (Eucalyptus nitens) residues for producción of second generation bioethanol2009Konferensbidrag (Övrigt vetenskapligt)
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