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Samikannu, Ajaikumar
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Publications (10 of 31) Show all publications
Samikannu, R., Shukla, S. K., Samikannu, A. & Mikkola, J.-P. (2019). Lutidinium-Based Ionic Liquids for Efficient Dissolution of Cellulose. New Journal of Chemistry, 43(5), 2299-2306
Open this publication in new window or tab >>Lutidinium-Based Ionic Liquids for Efficient Dissolution of Cellulose
2019 (English)In: New Journal of Chemistry, ISSN 1144-0546, E-ISSN 1369-9261, Vol. 43, no 5, p. 2299-2306Article in journal (Refereed) Published
Abstract [en]

Herein, we have studied the potential of lutidinium-based ILs (1-allyl-3,5-dimethylpyridinium chloride [3,5-ADMPy]Cl and 1-allyl-3,4-dimethylpyridinium chloride [3,4-ADMPy]Cl) in the dissolution of cellulose, and their structures were confirmed by 1H and 13C NMR spectra, respectively. [3,5-ADMPy]Cl exhibited the highest capacity in cellulose dissolution. In fact, it dissolved 20 wt% of cellulose within 12 min and 26 wt% of cellulose in 35 min at 118 °C. The crystallinity and morphology of native and regenerated cellulose were characterised by X-ray diffraction (XRD), scanning electron microscopy (SEM) and CP/MAS 13C NMR spectroscopy. These techniques clearly suggest that the crystallinity of cellulose is reduced upon treatment in lutidinium-based ILs. The thermogravimetric analysis (TGA) showed that regenerated cellulose had thermal stability close to that of native cellulose.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2019
Keywords
Cellulose dissolution, Ionic Liquids, X-ray diffraction, Cross polymerization/magic angle spinning C NMR, Thermogravimetric analysis, viscosity, scanning electron microscopy
National Category
Inorganic Chemistry
Identifiers
urn:nbn:se:umu:diva-154779 (URN)10.1039/C8NJ04698K (DOI)000459581000027 ()
Projects
Bio4Energy
Available from: 2019-01-02 Created: 2019-01-02 Last updated: 2019-08-29Bibliographically approved
Samikannu, A., Konwar, L. J., Mäki-Arvela, P. & Mikkola, J.-P. (2019). Renewable N-doped active carbons as efficient catalysts for direct synthesis of cyclic carbonates from epoxides and CO2. Applied Catalysis B: Environmental, 241, 41-51
Open this publication in new window or tab >>Renewable N-doped active carbons as efficient catalysts for direct synthesis of cyclic carbonates from epoxides and CO2
2019 (English)In: Applied Catalysis B: Environmental, ISSN 0926-3373, E-ISSN 1873-3883, Vol. 241, p. 41-51Article in journal (Refereed) Published
Abstract [en]

In the spirit of green chemistry and greenhouse gas mitigation, we explore herein the chemical utilization of CO2 upon synthesis of cyclic carbonates over N-doped activated carbons. The N-doped carbocatalysts were obtained from inexpensive N-rich bio-waste precursors and characterized by standard techniques (N2 physisorption, chemisorption, XPS, SEM, TEM, XRD, FT-IR and Micro-Raman spectroscopy). The materials exhibited excellent catalytic activity for direct carbonation of epoxides with CO2 to cyclic carbonates (yields upto 99%) under solvent free, moderate temperature (100–150 °C) and low CO2 pressure (5–50 bar) conditions. The observed catalytic activity of the N-doped carbocatalysts was attributed to the Lewis basic sites originating from pyridinic, pyridonic, and quaternary N-sites capable of activating the CO2 molecule. While control experiments with multiwalled carbon nanotubes (MWCNT) or commercial activated carbon, failed to produce cyclic carbonates due to lack of active (basic) sites. In terms of the catalytic performance, the N-doped carbocatalysts presenting a high porosity (634–1316 m2/g) and high levels of pyridinic (33%) and quaternary N-doping (30%), (i.e. CA500 and MA500), exhibited the highest activity and selectivity (TOF, conversion and cyclic carbonate yields upto 99% in 5–15 h). Most importantly, these materials demonstrated good operational stability and reusability.

Place, publisher, year, edition, pages
Elsevier, 2019
Keywords
CO2 utilization, N-doped carbons, cyclic carbonates, metal free catalysis
National Category
Organic Chemistry
Identifiers
urn:nbn:se:umu:diva-151687 (URN)10.1016/j.apcatb.2018.09.019 (DOI)000449444000005 ()2-s2.0-85053212900 (Scopus ID)
Projects
Bio4Energy
Funder
The Kempe Foundations
Available from: 2018-09-10 Created: 2018-09-10 Last updated: 2019-10-16Bibliographically approved
Durgadevi, G., Samikannu, A., Chandran, M., Kuppusamy, M. R. & Dinakaran, K. (2019). Synthesis and characterization of CdS nanoparticle anchored Silica-Titania mixed Oxide mesoporous particles: Efficient photocatalyst for discoloration of textile effluent. International Journal of Nano Dimension, 10(3), 272-280
Open this publication in new window or tab >>Synthesis and characterization of CdS nanoparticle anchored Silica-Titania mixed Oxide mesoporous particles: Efficient photocatalyst for discoloration of textile effluent
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2019 (English)In: International Journal of Nano Dimension, ISSN 2008-8868, E-ISSN 2228-5059, Vol. 10, no 3, p. 272-280Article in journal (Refereed) Published
Abstract [en]

An efficient photocatalyst consisting of CdS nanoparticle dispersed mesoporous silica-titania was prepared using amphiphilic triblock copolymer P123 as template and silica-titania sol-gel precursors. The CdS nanoparticle was incorporated into silica-titania mesoporous nanosturctures by post impregnation method. The synthesized catalyst has been characterized by FTIR, TEM, SEM, and EDAX analysis. The CdS nanoparticles incorporated silica-titania mesoporous particles exhibited an enhanced light harvesting, large surface area and excellent photocatalytic activity. Photocatalytic degradation experiments on methyleneblue solution at different pH of the medium revealed that, the catalyst ST0.5CdS0.2 is more effective in basic medium with a degradation efficiency of 98%. In addition, the catalyst is also tested for dye degradation against a raw textile dye effluent containing multiple dye molecules, and their results indicated that the raw effluent can be decolorized within 90min using ST0.5CdS0.2 catalyst.

Place, publisher, year, edition, pages
the Tonekabon branch of the Islamic Azad University, 2019
Keywords
Cadmium Sulfide, Mesoporous Material, Methylene Blue, Photocatalyst, Photodegradation, Silica-Titania, Textile Effluent
National Category
Materials Chemistry
Identifiers
urn:nbn:se:umu:diva-159839 (URN)000466139300005 ()
Projects
Bio4Energy
Available from: 2019-06-11 Created: 2019-06-11 Last updated: 2019-09-02Bibliographically approved
Konwar, L. J., Samikannu, A., Mäki-Arvela, P. & Mikkola, J.-P. (2018). Efficient C-C coupling of bio-based furanics and carbonyl compounds to liquid hydrocarbon precursors over lignosulfonate derived acidic carbocatalysts. Catalysis Science & Technology, 8(9), 2449-2459
Open this publication in new window or tab >>Efficient C-C coupling of bio-based furanics and carbonyl compounds to liquid hydrocarbon precursors over lignosulfonate derived acidic carbocatalysts
2018 (English)In: Catalysis Science & Technology, ISSN 2044-4753, E-ISSN 2044-4761, Vol. 8, no 9, p. 2449-2459Article in journal (Refereed) Published
Abstract [en]

This paper demonstrates the catalytic potential of novel Na-lignosulfonate (LS) derived meso/macroporous solid protonic acids upon C–C coupling of bio-based furanics and carbonyl compounds. The materials demonstrated catalytic activity for solventless hydroxyalkylation/alkylation (HAA) of 2-methylfuran with furfural, acetone, butanal, cyclohexanone, levulinic acid and α-angelica lactone under mild reaction conditions (50–60 °C) producing branched-chain C12–C16 hydrocarbon precursors in yields approaching 96%. Moreover, the carbon materials exhibiting high total acidity (6–6.4 mmol g−1) outperformed sulfonic acid resins (Amberlyst®70, Amberlite®IR120 and LS resin), zeolites and liquid acids (p-toluenesulfonic acid, acetic acid and phenol). In fact, the most active carbocatalyst (60LS40PS350H+) exhibited the same turnover frequency as p-toluenesulfonic acid (186 h−1) upon furfural conversion but with an improved HAA product yield (up to 88%) and reusability, maintaining 98% of its original activity up to seven reaction cycles. The observed catalytic activity and operational stability of the LS derived acidic carbocatalysts were attributed to the strongly Brønsted acidic –SO3H groups covalently incorporated into their structural carbon framework and the promotional effects of hydrophilic surface functional groups (–COOH and –OH) favoring adsorption of oxygenated reactant molecules.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2018
National Category
Organic Chemistry
Identifiers
urn:nbn:se:umu:diva-146304 (URN)10.1039/C7CY02601C (DOI)000433163900021 ()
Projects
Bio4Energy
Available from: 2018-04-04 Created: 2018-04-04 Last updated: 2019-08-29Bibliographically approved
Verziu, M., Tirsoaga, A., Cojocaru, B., Bucur, C., Tudora, B., Richel, A., . . . Mikkola, J. P. (2018). Hydrogenolysis of lignin over Ru-based catalysts: the role of the ruthenium in a lignin fragmentation process. Molecular Catalysis, 450, 65-76
Open this publication in new window or tab >>Hydrogenolysis of lignin over Ru-based catalysts: the role of the ruthenium in a lignin fragmentation process
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2018 (English)In: Molecular Catalysis, ISSN 2468-8231, Vol. 450, p. 65-76Article in journal (Refereed) Published
Abstract [en]

The catalytic performances of two different classes of catalysts containing nickel or/and ruthenium as the active sites were studied in the depolymerisation of lignin isolated from Miscanthus×giganteus. The catalysts were prepared either by coprecipitation (ie, (RuNiMgAlO)x, (RuNiAlO)x, (NiAlO)x, (NiMgAlO)x) or by wet impregnation (ie, Ru/Al2O3) and characterized by nitrogen physisorption (BET), XRD, XPS, NH3-TPD, Raman and H2-TPR techniques. The experimental results indicate that the presence of ruthenium led to dimers as dominant products.

Place, publisher, year, edition, pages
Elsevier, 2018
Keywords
lignin, hydrogenolysis, heterogeneous catalysts, Ru-based catalysts
National Category
Organic Chemistry
Identifiers
urn:nbn:se:umu:diva-146057 (URN)10.1016/j.mcat.2018.03.004 (DOI)000431158400008 ()
Projects
Bio4Energy
Available from: 2018-03-28 Created: 2018-03-28 Last updated: 2019-09-02Bibliographically approved
Konwar, L. J., Samikannu, A., Mäki-Arvela, P., Boström, D. & Mikkola, J.-P. (2018). Lignosulfonate-based macro/mesoporous solid protonic acids for acetalization of glycerol to bio-additives. Applied Catalysis B: Environmental, 220, 314-323
Open this publication in new window or tab >>Lignosulfonate-based macro/mesoporous solid protonic acids for acetalization of glycerol to bio-additives
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2018 (English)In: Applied Catalysis B: Environmental, ISSN 0926-3373, E-ISSN 1873-3883, Vol. 220, p. 314-323Article in journal (Refereed) Published
Abstract [en]

The enclosed paper introduces a novel, scalable and environmentally benign process for making strongly acidic solid meso/macroporous carbon catalysts from Na-lignosulfonate (LS), a byproduct from sulfite pulping. Ice-templated LS was converted to strongly acidic macro/mesoporous solid protonic acids via mild pyrolysis (350–450 °C) and ion/H+ exchanging technique. The synthesized materials were extensively characterized by FT-IR, Raman, XRD, XPS, TGA, FE-SEM, TEM and N2-physisorption methods. These LS derived materials exhibited a macro/mesoporous and highly functionalized heteroatom doped (O, S) carbon structure with large amounts of surface OH, COOH and SO3H groups similar to the sulfonated carbon materials. Further, these carbon materials showed excellent potential as solid acid catalysts upon acetalization of glycerol with various bio-based aldehydes and ketones (acetone, methyl levulinate and furfural), easily outperforming the commercial acid exchange resins (Amberlite® IR120 and Amberlyst® 70). Most importantly, the optimum LS catalyst exhibiting a large specific surface area demonstrated exceptional potential for continuous solketal production (liquid phase atmospheric pressure operation) maintaining its activity (glycerol conversion ≥ 91%) and structural features even after 90 h time on stream.

Place, publisher, year, edition, pages
Amsterdam: Elsevier, 2018
Keywords
Solid sulfonic acids, Glycerol acetalization, Bio-additives, Solketal, Lignosulfonate
National Category
Chemical Sciences
Identifiers
urn:nbn:se:umu:diva-139656 (URN)10.1016/j.apcatb.2017.08.061 (DOI)000412957200030 ()
Projects
Bio4Energy
Available from: 2017-09-20 Created: 2017-09-20 Last updated: 2019-08-29Bibliographically approved
Bukhanko, N., Schwarz, C., Samikannu, A., Ngoc Pham, T., Siljebo, W., Wärnå, J., . . . Mikkola, J.-P. (2017). Gas phase synthesis of isopropyl chloride from isopropanol and HCl over alumina and flexible 3-D carbon foam supported catalysts. Applied Catalysis A: General, 542(25), 212-225
Open this publication in new window or tab >>Gas phase synthesis of isopropyl chloride from isopropanol and HCl over alumina and flexible 3-D carbon foam supported catalysts
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2017 (English)In: Applied Catalysis A: General, ISSN 0926-860X, E-ISSN 1873-3875, Vol. 542, no 25, p. 212-225Article in journal (Refereed) Published
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.

Place, publisher, year, edition, pages
Elsevier, 2017
Keywords
Isopropyl chloride; Heterogeneous catalysis; Isopropanol; Hydrochlorination; Zinc chloride; Alumina oxide; Carbon foam; Highly porous catalyst
National Category
Chemical Sciences
Identifiers
urn:nbn:se:umu:diva-127043 (URN)10.1016/j.apcata.2017.05.013 (DOI)000405765200019 ()
Projects
Bio4Energy
Available from: 2016-10-26 Created: 2016-10-26 Last updated: 2019-09-02Bibliographically approved
Kocík, J., Samikannu, A., Bourajoini, H., Pham, T. N., Mikkola, J.-P., Hájek, M. & Čapek, L. (2017). Screening of active solid catalysts for esterification of tall oil fatty acids with methanol. Journal of Cleaner Production, 155(1), 34-38
Open this publication in new window or tab >>Screening of active solid catalysts for esterification of tall oil fatty acids with methanol
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2017 (English)In: Journal of Cleaner Production, ISSN 0959-6526, E-ISSN 1879-1786, Vol. 155, no 1, p. 34-38Article in journal (Refereed) Published
Abstract [en]

The paper is focused on the description of the activity/selectivity of mesoporous silica based materials loaded with various types of active species in the esterification of tall oil free fatty acids. The metals such as aluminium, molybdenum, gallium and zinc, including their combinations were impregnated on the mesoporous silica, which was tested in esterification reaction. All these catalysts preserved its tall oil free fatty conversion in the first and the second catalytic cycles. However, while only insignificant amount of gallium or molybdenum was lost from the solid catalyst into the liquid phases, zinc leached from every studied solid catalyst. In contrast to impregnated gallium on mesoporous silica, which exhibited higher acidity and higher tall oil free fatty acids conversion in the first catalytic cycle, but its value was not preserved in the second catalytic test.

Place, publisher, year, edition, pages
Elsevier, 2017
Keywords
Esterification, Biodiesel, TOFA, Mixed oxides, SBA-15, Al-SBA-15
National Category
Chemical Process Engineering Biocatalysis and Enzyme Technology
Identifiers
urn:nbn:se:umu:diva-128682 (URN)10.1016/j.jclepro.2016.09.174 (DOI)000401887700005 ()2-s2.0-85008674705 (Scopus ID)
Projects
Bio4Energy
Available from: 2016-12-12 Created: 2016-12-12 Last updated: 2019-08-30Bibliographically approved
Ngoc Pham, T., Samikannu, A., Rautio, A.-R., Juhasz, K. L., Konya, Z., Wärnå, J., . . . Mikkola, J.-P. (2016). Catalytic Hydrogenation of d-Xylose Over Ru Decorated Carbon Foam Catalyst in a SpinChem® Rotating Bed Reactor. Topics in catalysis, 59(13-14), 1165-1177
Open this publication in new window or tab >>Catalytic Hydrogenation of d-Xylose Over Ru Decorated Carbon Foam Catalyst in a SpinChem® Rotating Bed Reactor
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2016 (English)In: Topics in catalysis, ISSN 1022-5528, E-ISSN 1572-9028, Vol. 59, no 13-14, p. 1165-1177Article in journal (Refereed) Published
Abstract [en]

In this work the activity of ruthenium decorated carbon foam (Ru/CF) catalyst was studied in three phase hydrogenation reaction of d-xylose to d-xylitol. The developed catalyst was characterized by using scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, inductively coupled plasma optical emission spectrometry and nitrogen adsorption–desorption measurement. Kinetic measurements were carried out in a laboratory scale pressurized reactor (Parr®) assisted by SpinChem® rotating bed reactor (SRBR), at pre-defined conditions (40–60 bar H2 and 100–120 °C). The study on the influence of reaction conditions showed that the conversion rate and selectivity of hydrogenation reaction of d-xylose was significantly affected by temperature. These results have been proved by a competitive kinetics model which was found to describe the behavior of the novel system (Ru/CF catalyst used together with the SRBR) very well. Besides, it was revealed that the catalytic activity as well as the stability of our Ru/CF-SRBR is comparable with the commercial ruthenium decorated carbon catalyst (Ru/AC) under identical reaction conditions. Moreover, all steps from catalyst preparation and catalyst recycling as well as catalytic testing can be performed in an easy, fast and elegant manner without any loss of materials. Briefly, the developed Ru/CF catalyst used together with the SRBR could be used an excellent alternative for the conventional Raney nickel catalyst in a slurry batch reactor and offers an attractive concept with obvious industrial applicability.

Place, publisher, year, edition, pages
New York: Springer, 2016
Keywords
d-xylose, d-xylitol, Ruthenium, Carbon foam, SpinChem, Rotating bed reactor
National Category
Chemical Sciences
Identifiers
urn:nbn:se:umu:diva-122090 (URN)10.1007/s11244-016-0637-4 (DOI)000381158900010 ()
Projects
Bio4Energy
Available from: 2016-06-15 Created: 2016-06-15 Last updated: 2019-09-02Bibliographically approved
Bukhanko, N., Wärnå, J., Samikannu, A. & Mikkola, J.-P. (2016). Kinetic modeling of gas phase synthesis of ethyl chloride from ethanol and HCl in fixed bed reactor. Chemical Engineering Science, 142, 310-317
Open this publication in new window or tab >>Kinetic modeling of gas phase synthesis of ethyl chloride from ethanol and HCl in fixed bed reactor
2016 (English)In: Chemical Engineering Science, ISSN 0009-2509, E-ISSN 1873-4405, Vol. 142, p. 310-317Article in journal (Refereed) Published
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.

Keywords
Ethyl chloride, Kinetic modeling, Gas-phase reaction, Heterogeneous catalysis
National Category
Chemical Sciences
Identifiers
urn:nbn:se:umu:diva-114093 (URN)10.1016/j.ces.2015.12.005 (DOI)000369068500027 ()
Projects
Bio4Energy
Available from: 2016-01-13 Created: 2016-01-13 Last updated: 2019-08-29Bibliographically approved
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