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Samikannu, Ajaikumar
Alternative names
Publications (10 of 48) Show all publications
Mariyaselvakumar, M., Kadam, G. G., Saha, A., Samikannu, A., Mikkola, J.-P., Ganguly, B., . . . Konwar, L. J. (2024). Halogenated melamine formaldehyde polymers: Efficient, robust and cost-effective bifunctional catalysts for continuous production of cyclic carbonates via. CO2-epoxide cycloaddition. Applied Catalysis A: General, 675, Article ID 119634.
Open this publication in new window or tab >>Halogenated melamine formaldehyde polymers: Efficient, robust and cost-effective bifunctional catalysts for continuous production of cyclic carbonates via. CO2-epoxide cycloaddition
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2024 (English)In: Applied Catalysis A: General, ISSN 0926-860X, E-ISSN 1873-3875, Vol. 675, article id 119634Article in journal (Refereed) Published
Abstract [en]

Halogenated porous melamine polymers were demonstrated as an efficient catalyst for CO2-epoxide cycloaddition, selectively (>99%) producing C3-C12 cyclic carbonates in excellent yields (upto 99%) under solvent and co-catalyst free conditions. The halogenated polymers outperformed benchmark catalysts incorporating only basic (N-doped carbon, ZIF-8, N-rich melamine polymer) or nucleophilic (TBAB, KI) sites. The superior catalytic performance of these inexpensive polymers was attributed to their unique surface chemistry incorporating abundant, stable basic N sites (amine N and protonated N) and nucleophilic (Cl-, Br- or I-) that enabled simultaneous activation of both epoxide and CO2 molecule (supported by kinetic and DFT studies). Further, among halogenated polymers a Br- containing material (PMFBr) presented highest activity owing to its balanced CO2-philicity and strong nucleophilicity. Most importantly, PMFBr was robust, reusable and maintained stable performance for continuous production of C3-C4 cyclic carbonate (120 oC, 0.3-0.83 h-1 WHSVepoxide and 15 bar) in a fixed-bed reactor during 60-190 h TOS.

Place, publisher, year, edition, pages
Elsevier, 2024
Keywords
CO2 utilization, Cyclic carbonate, Bifunctional catalyst, Continuous cyclic carbonate synthesis, Porous melamine formaldehyde polymer, DFT
National Category
Chemical Sciences
Identifiers
urn:nbn:se:umu:diva-221358 (URN)10.1016/j.apcata.2024.119634 (DOI)2-s2.0-85186488606 (Scopus ID)
Available from: 2024-02-21 Created: 2024-02-21 Last updated: 2024-03-13Bibliographically approved
Samikannu, A., Mikkola, J.-P., Tirsoaga, A., Tofan, V., Fierascu, R. C., Richel, A. & Nicolae Verziu, M. (2024). The activation of C–O bonds in lignin Miscanthus over acidic heterogeneous catalysts: towards lignin depolymerisation to monomer units. Biomass Conversion and Biorefinery, 14(8), 9723-9737
Open this publication in new window or tab >>The activation of C–O bonds in lignin Miscanthus over acidic heterogeneous catalysts: towards lignin depolymerisation to monomer units
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2024 (English)In: Biomass Conversion and Biorefinery, ISSN 2190-6815, E-ISSN 2190-6823, Vol. 14, no 8, p. 9723-9737Article in journal (Refereed) Published
Abstract [en]

One-pot depolymerisation of lignin, extracted from Miscanthus plants under acidic (formic acid lignin, FAL) or basic (ammonia lignin, AL) conditions, over Ni- and/or Nb-doped SBA-15, was the subject of this study. The aforementioned acid catalysts prepared by sol–gel method were characterized by SEM–EDX, ATR-FTIR, Raman, XRD, N2 adsorption/desorption isotherms, CO2-TPD and NH3-TPD techniques. The increase in acidity due to the insertion of Nb into the SBA-15 structure promoted the selective cleavage of β–O–4 from ammonia lignin, leading to aromatic monomer yields up to 22 wt% in 6 h at 180 °C under 50 atm H2. The catalytic performances of Ni-Nb-SBA-15 as well as its stability were influenced by the chemical composition of the lignin sample as results of its extraction from the Miscanthus plant.

Place, publisher, year, edition, pages
Springer, 2024
Keywords
Lignin Miscanthus, Hydrogenolysis, Monomers, Methanol, Synergistic efect
National Category
Chemical Sciences
Identifiers
urn:nbn:se:umu:diva-198249 (URN)10.1007/s13399-022-03061-4 (DOI)000828950800001 ()2-s2.0-85134654307 (Scopus ID)
Funder
Bio4EnergyKnut and Alice Wallenberg FoundationThe Kempe Foundations
Available from: 2022-07-24 Created: 2022-07-24 Last updated: 2024-05-10Bibliographically approved
Adeniyi, O., Osmanaj, B., Manavalan, G., Samikannu, A., Mikkola, J.-P., Avni, B., . . . Tesfalidet, S. (2023). Engineering of layered iron vanadate nanostructure for electrocatalysis: simultaneous detection of methotrexate and folinic acid in blood serum. Electrochimica Acta, Article ID 142538.
Open this publication in new window or tab >>Engineering of layered iron vanadate nanostructure for electrocatalysis: simultaneous detection of methotrexate and folinic acid in blood serum
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2023 (English)In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, article id 142538Article in journal (Refereed) Published
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.

Place, publisher, year, edition, pages
Elsevier, 2023
Keywords
Iron vanadate, voltammetric sensor, electrocatalysts, therapeutic drug monitoring, methotrexate, folinic acid
National Category
Analytical Chemistry
Identifiers
urn:nbn:se:umu:diva-208011 (URN)10.1016/j.electacta.2023.142538 (DOI)001007246800001 ()2-s2.0-85159099130 (Scopus ID)
Funder
The Kempe FoundationsBio4Energy
Available from: 2023-05-08 Created: 2023-05-08 Last updated: 2023-11-06Bibliographically approved
Mani, M., Mariyaselvakumar, M., Samikannu, A., Panda, A. B., Konwar, L. J. & Mikkola, J.-P. (2022). Continuous hydrocyclization of aqueous levulinic acid to γ-valerolactone over bi-functional Ru/NbOPO4/SBA-15 catalyst under mild conditions. Applied Catalysis A: General, 643, Article ID 118744.
Open this publication in new window or tab >>Continuous hydrocyclization of aqueous levulinic acid to γ-valerolactone over bi-functional Ru/NbOPO4/SBA-15 catalyst under mild conditions
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2022 (English)In: Applied Catalysis A: General, ISSN 0926-860X, E-ISSN 1873-3875, Vol. 643, article id 118744Article in journal (Refereed) Published
Abstract [en]

Herein, we demonstrate that surface acid-base properties have marked effect upon the performance (activity, selectivity and stability) of supported Ru catalysts upon tandem hydrocyclization (hydrogenation-dehydration) of aqueous levulinic acid. A mesoporous bi-functional Ru/NbOPO4/SBA-15 catalyst incorporating highly dispersed Ru sites and well balanced strong Brønsted acidic sites (optimum B/L and M+S/W ratio) was identified, which outperformed the benchmark monofuncational (Ru/SBA-15, Ru/MCM-41) and physically blended bi-functional catalysts (Ru catalysts mixed with acid co-catalysts e.g. NbOPO4/Amberlyst-15). Further, the catalyst also demonstrated remarkable stability in a fixed-bed reactor, maintaining steady activity and γ-valerolactone selectivity (72-86%) during ca. 300 h time on stream (10 bar, 90-100 oC), corroborating its industrial potential. The exceptional performance and durability of the bi-functional catalyst was attributed to the presence of well dispersed hydrothermally and chemically stable acid (NbOPO4) and redox (Ru) sites.

Place, publisher, year, edition, pages
Elsevier, 2022
Keywords
Tandem hydrocyclization, γ-valerolactone, Supported Ru-catalysts, Bi-functional catalyst, Flow chemistry, Catalyst deactivation
National Category
Chemical Sciences
Identifiers
urn:nbn:se:umu:diva-197463 (URN)10.1016/j.apcata.2022.118744 (DOI)000827290500001 ()2-s2.0-85133252862 (Scopus ID)
Available from: 2022-06-28 Created: 2022-06-28 Last updated: 2023-09-05Bibliographically approved
Ngoc Pham, T., Samikannu, A., Vincze, Z., Zettinig, P., Tesfalidet, S., Wågberg, T. & Mikkola, J.-P. (2022). Core–shell carbon nanofibers‐NiFe structure on 3D porous carbon foam: facilitating a promising trajectory toward decarbonizing energy production. Advanced sustainable systems, 6(12), Article ID 2200310.
Open this publication in new window or tab >>Core–shell carbon nanofibers‐NiFe structure on 3D porous carbon foam: facilitating a promising trajectory toward decarbonizing energy production
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2022 (English)In: Advanced sustainable systems, ISSN 2366-7486, Vol. 6, no 12, article id 2200310Article in journal (Refereed) Published
Abstract [en]

In this work, a low-cost, light-weight, highly efficient, and durable electrode in which NiFe-layered double hydroxide is electrodeposited on a carbon nanofiber (CNF) core supported on a carbon foam (CF) is introduced. The resulting 3D NiFe-CNFs-CF electrode shows excellent oxygen evolution reaction and hydrogen evolution reaction performance in alkaline media. When used as an anode and a cathode in the same cell, a current density of 10 mA cm−2 is achieved, at a cell voltage of 1.65 V. Moreover, good stability over a long testing time (50 h) is demonstrated. The ternary hybrid electrode gives rise to an excellent performance-to-weight ratio owing to its very low bulk density (≈34 mg cm−3) inherited from super lightweight components composed of CF and CNFs. The developed electrode can potentially be used in large-scale alkaline water electrolysis, in facilities such as offshore hydrogen production platforms, which can complement the variable renewable energy production of wind farms through hydrogen storage and fuel cells.

Place, publisher, year, edition, pages
Wiley-VCH Verlagsgesellschaft, 2022
National Category
Chemical Sciences
Identifiers
urn:nbn:se:umu:diva-200895 (URN)10.1002/adsu.202200310 (DOI)000879600200001 ()2-s2.0-85141445618 (Scopus ID)
Funder
Swedish Energy Agency, 45419‐1The Kempe Foundations
Available from: 2022-11-08 Created: 2022-11-08 Last updated: 2022-12-30Bibliographically approved
Konwar, L. J., Oliani, B., Samikannu, A., Canu, P. & Mikkola, J.-P. (2022). Efficient hydrothermal deoxygenation of tall oil fatty acids into n-paraffinic hydrocarbons and alcohols in the presence of aqueous formic acid. Biomass Conversion and Biorefinery, 12(1), 51-62
Open this publication in new window or tab >>Efficient hydrothermal deoxygenation of tall oil fatty acids into n-paraffinic hydrocarbons and alcohols in the presence of aqueous formic acid
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2022 (English)In: Biomass Conversion and Biorefinery, ISSN 2190-6815, E-ISSN 2190-6823, Vol. 12, no 1, p. 51-62Article in journal (Refereed) Published
Abstract [en]

Hydrothermal deoxygenation of tall oil fatty acids (TOFA) was investigated in the presence of aqueous formic acid (0.5–7.5 wt%) as a H2 donor in the presence of subcritical H2O pressure (569–599 K). Pd and Ru nanoparticles supported on carbon (5% Pd/CSigma, 5% Ru/CSigma, 10% Pd/CO850_DP, and 5% Ru/COPcomm_DP) were found to be efficient catalysts for deoxygenation of TOFA. The reaction pathway was mainly influenced by the concentration of formic acid and the catalyst. In case of Pd catalysts, in the presence of 0–2.5 wt% formic acid, decarboxylation was the dominant pathway producing n-paraffinic hydrocarbons with one less carbon atom (heptadecane yield up to 94 wt%), while with 5–7.5% formic acid, a hydrodeoxygenation/hydrogenation mechanism was favored producing C18 deoxygenation products octadecanol and octadecane as the main products (yields up to 70 wt%). In contrast, Ru catalysts produced a mixture of C5-C20 (n-and iso-paraffinic) hydrocarbons via decarboxylation, cracking and isomerization (up to 58 wt% C17 yield and total hydrocarbon yield up to 95 wt%) irrespective of formic acid concentration. Kinetic studies showed that the rates of deoxygenation displayed Arrhenius type behavior with apparent activation energies of 134.44 ± 31.36 kJ/mol and 148.92 ± 3.66 kJ/mol, for the 5% Pd/CSigma and 5% Ru/CSigma catalyst, respectively. Furthermore, the experiments with glycerol tristearate, rapeseed oil, sunflower oil, rapeseed biodiesel, and hydrolyzed rapeseed oil produced identical products confirming the versatility of the aforementioned catalytic systems for deoxygenation of C18 feedstocks.

Place, publisher, year, edition, pages
Springer, 2022
Keywords
Hydrothermal deoxygnation, Supported carbon catalysts, Transfer hydrogenation, Green diesel
National Category
Chemical Process Engineering Organic Chemistry Biocatalysis and Enzyme Technology
Identifiers
urn:nbn:se:umu:diva-176571 (URN)10.1007/s13399-020-01103-3 (DOI)000587192400001 ()2-s2.0-85095438534 (Scopus ID)
Projects
Bio4Energy
Funder
Bio4EnergyWallenberg FoundationsThe Kempe Foundations
Available from: 2020-11-09 Created: 2020-11-09 Last updated: 2022-07-12Bibliographically approved
Jogi, R., Samikannu, A., Mäki-Arvela, P., Virtanen, P., Hemming, J., Smeds, A., . . . Mikkola, J.-P. (2022). Liquefaction of Lignocellulosic Biomass into Phenolic Monomers and Dimers Over Multifunctional Pd/Nbopo4 Catalyst.
Open this publication in new window or tab >>Liquefaction of Lignocellulosic Biomass into Phenolic Monomers and Dimers Over Multifunctional Pd/Nbopo4 Catalyst
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2022 (English)Manuscript (preprint) (Other academic)
Abstract [en]

For the first time, a tandem catalytic material namely 5 wt. % Pd/NbOPO 4 was utilized in the depolymerization of wood in supercritical-ethanol under low initial-hydrogen pressure. The experiments were conducted under various experimental conditions, wood fractionation was executed with fresh, and acetone extracted birch. A comprehensive analysis was performed to elucidate the dissolution efficiency and achieved product distribution. The results indicated fresh birch, 34 wt. % of lignin monomer yield with 84 wt. % delignification efficiency were obtained while extracted wood, 35 wt. % of lignin monomer yield with 78 wt. % delignification efficiency was achieved. The total lignin monomer content extracted from the fresh birch is composed of 76.9 wt. % of dimethoxyphenols and 16.5 wt. % of monomers with the guaiacol structure. Among the dimethoxyphenols, major homosyringaldehyde (61.9 wt. %). Where extracted wood, 93.2 wt. % of dimethoxyphenols (63.6 wt. % homosyringaldehyde) and guaiacol-monomers (6.8 wt. %). It was concluded that the depolymerization occurred via breaking of the ether bonds in lignin, including ether hydrolysis by Lewis acid sites over the solid acid catalyst and with subsequent deoxygenation of monophenols over Pd. In addition, an extraction process was proposed to extract the aromatic fraction from the obtained biocrude.

National Category
Chemical Sciences
Identifiers
urn:nbn:se:umu:diva-198313 (URN)10.2139/ssrn.4093291 (DOI)
Available from: 2022-07-28 Created: 2022-07-28 Last updated: 2022-07-29
Mukesh, C., Sarmad, S., Samikannu, A., Nikjoo, D., Siljebo, W. & Mikkola, J.-P. (2022). Pore size-excluded low viscous porous liquids for CO2 sorption at room temperature and thermodynamic modeling study. Journal of Molecular Liquids, 356, Article ID 119046.
Open this publication in new window or tab >>Pore size-excluded low viscous porous liquids for CO2 sorption at room temperature and thermodynamic modeling study
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2022 (English)In: Journal of Molecular Liquids, ISSN 0167-7322, E-ISSN 1873-3166, Vol. 356, article id 119046Article in journal (Refereed) Published
Abstract [en]

Herein, we report porous ionic liquids (type-III) designed to utilize microporous ZIF-8 moieties with functional ionic liquids such as 8-(2-methoxyethyl)-1,8-Diazabicyclo[5.4.0]undec-7-en-8-ium, Bis(trifluoromethane)sulfonamide ([MEDBU][TFSI] and Trioctylammonium 4-para-tert-butylbenzoiate [TOAH][PTBBA]). The prepared materials were thoroughly characterized by means of XRD, FT-IR, SEM, TEM, BET, TGA, DSC and viscometry techniques. The idea of combining the intrinsic properties of ionic liquids with microporous architecture to prepare porous ionic liquids yields promising fluidic materials that have received attention in industrial applications such as gas sorption and separation etc. The prepared porous ionic liquids possess unique physico-chemical properties such as low viscosity, high thermal stability, low vapor pressure, reusability and their fluidic nature renders the materials suitable for CO2 capture. Herein introduced porous ionic liquids (ILs) showed enhanced CO2 uptake (0.92 mmol/g in [TOAH][PTBBA]-Z100 and 1.16 mmol/g in [MEDBU][TFSI]-Z200), or in other words, 15–47% higher sorption capacity compared to neat ionic liquids. This concept overcomes the drawbacks of highly viscous ILs and their limited CO2 sorption capacity. Thermodynamic modeling further demonstrated that the enthalpy of sorption is only −9.99 kJ mol−1, indicating that significantly less energy is required for regeneration. This is promising for the potential use of these fluidic materials in continuous separation processes on an industrial scale, as a better alternative to the existing hazardous amine scrubbing.

Place, publisher, year, edition, pages
Elsevier, 2022
National Category
Physical Chemistry Materials Chemistry
Identifiers
urn:nbn:se:umu:diva-194108 (URN)10.1016/j.molliq.2022.119046 (DOI)000799182800017 ()2-s2.0-85128835880 (Scopus ID)
Funder
Bio4EnergyThe Kempe FoundationsKnut and Alice Wallenberg Foundation
Available from: 2022-04-25 Created: 2022-04-25 Last updated: 2023-09-05Bibliographically approved
Ngoc Pham, T., Samikannu, A., Tesfalidet, S., Wågberg, T. & Mikkola, J.-P. (2021). NiCo Nanoneedles on 3D Carbon Nanotubes/Carbon Foam Electrode as an Efficient Bi-Functional Catalyst for Electro-Oxidation of Water and Methanol. Catalysts, 11(4), Article ID 500.
Open this publication in new window or tab >>NiCo Nanoneedles on 3D Carbon Nanotubes/Carbon Foam Electrode as an Efficient Bi-Functional Catalyst for Electro-Oxidation of Water and Methanol
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2021 (English)In: Catalysts, E-ISSN 2073-4344, Vol. 11, no 4, article id 500Article in journal (Refereed) Published
Abstract [en]

In this study, we report a 3D structured carbon foam electrode assembled from a bi-functional NiCo catalyst, carbon nanotubes (CNT), and a monolith 3D structured carbon foam (CF) as a highly active and stable electrode for oxygen evolution reaction (OER) and methanol oxidation reaction (MOR). When the NiCo@CNTs/CF electrode was used as an anode in OER, after the anodization step, the electrode required a small overpotential of 320 mV to reach the current density of 10 mA cm−2 and demonstrated excellent stability over a long testing time (total 30 h) in 1 M KOH. The as-prepared NiCo@CNTs/CF electrode also exhibited a good performance towards methanol oxidation reaction (MOR) with high current density, 100 mA cm−2 at 0.6 V vs. Ag/AgCl, and good stability in 1 M KOH plus 0.5 M CH3OH electrolyte. The NiCo@CNTs/CF catalyst/electrode provides a potential for application as an anode in water electrolysis and direct methanol fuel cells.

Place, publisher, year, edition, pages
MDPI, 2021
Keywords
NiCo bi-functional catalyst, CNTs, carbon foam, OER, MOR
National Category
Materials Chemistry
Identifiers
urn:nbn:se:umu:diva-182708 (URN)10.3390/catal11040500 (DOI)000642861000001 ()2-s2.0-85104110259 (Scopus ID)
Available from: 2021-05-03 Created: 2021-05-03 Last updated: 2023-09-05Bibliographically approved
Samikannu, A., Konwar, L. J., Rajendran, K., Lee, C. C., Shchukarev, A., Virtanen, P. & Mikkola, J.-P. (2020). Highly dispersed NbOPO4/SBA-15 as a versatile acid catalyst upon production of renewable jet-fuel from bio-based furanics via hydroxyalkylation-alkylation (HAA) and hydrodeoxygenation (HDO) reactions. Applied Catalysis B: Environmental, 272, Article ID 118987.
Open this publication in new window or tab >>Highly dispersed NbOPO4/SBA-15 as a versatile acid catalyst upon production of renewable jet-fuel from bio-based furanics via hydroxyalkylation-alkylation (HAA) and hydrodeoxygenation (HDO) reactions
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2020 (English)In: Applied Catalysis B: Environmental, ISSN 0926-3373, E-ISSN 1873-3883, Vol. 272, article id 118987Article in journal (Refereed) Published
Abstract [en]

Herein, we report the synthesis of a highly active and mesoporous Brønsted acidic NbOPO4/SBA-15 catalyst. The prepared catalysts were thoroughly characterized by means of analytical techniques such as XRD, FT-IR, XPS, NH3-TPD, SEM-EDS, TEM, TGA, 31P-MAS-NMR and N2-physisorption. The H3PO4 free deposition method was found to be effective for preserving the structure of Silica based carrier. In terms of catalytic performance, these materials demonstrated high activity upon C-C coupling of 2-methyl furan with carbonyl compounds and outperforming bulk NbOPO4, Nb2O5/SBA-15 and traditional solid acid catalysts (Al-MCM-41, Si/Al and H-ZSM-5). The NbOPO4/SBA-15 catalysts were stable and maintained high activity upon reuse and continuous operation (∼65 h). Furthermore, the Pd loaded counterparts (Pd/NbOPO4/SBA-15 and Pd/Nb2O5/SBA-15) also functioned as bifunctional catalysts and exhibited excellent activity upon subsequent hydrodeoxygenation of C-C coupling products. Most importantly, in terms of jet-fuel range hydrocarbons selectivity, these catalysts outperformed monofunctional Pd/carbon and aluminosilicate based bifunctional catalysts.

Place, publisher, year, edition, pages
Elsevier, 2020
Keywords
Supported solid acid catalysts, Mesoporous NbOPO4, C-C coupling, Hydrodeoxygenation, Jet-Fuel
National Category
Organic Chemistry Other Chemical Engineering Chemical Process Engineering Inorganic Chemistry Biocatalysis and Enzyme Technology
Identifiers
urn:nbn:se:umu:diva-170334 (URN)10.1016/j.apcatb.2020.118987 (DOI)000533148700026 ()2-s2.0-85084203311 (Scopus ID)
Projects
Bio4Energy
Funder
Bio4Energy
Available from: 2020-05-04 Created: 2020-05-04 Last updated: 2023-08-25Bibliographically approved
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