New Opportunity for Carbon-Supported Ni-based Electrocatalysts: Gas-Phase CO2 Methanation

Liliana P.L. Gonçalves; Alexey Serov; Geoffrey McCool; Mikaela Dicome; Juliana P.S. Sousa; O. Salomé G.P. Soares; Oleksandr Bondarchuk; Dmitri Y. Petrovykh; Oleg I. Lebedev; M. Fernando R. Pereira; Yury V. Kolen'ko

doi:10.1002/cctc.202101284

New Opportunity for Carbon-Supported Ni-based Electrocatalysts: Gas-Phase CO₂ Methanation

Liliana P.L. Gonçalves, Alexey Serov, Geoffrey McCool, Mikaela Dicome, Juliana P.S. Sousa, O. Salomé G.P. Soares, Oleksandr Bondarchuk, Dmitri Y. Petrovykh, Oleg I. Lebedev, M. Fernando R. Pereira, Yury V. Kolen'ko

Energy Storage and Conversion Manufactur

Research output: Contribution to journal › Article › peer-review

8 Scopus citations

Abstract

The cost-effectiveness and excellent performance of conductive-carbon-supported Ni-based electrocatalysts make them attractive materials for hydrogen oxidation and evolution reactions. However, they were previously unused in gas-phase hydrogenation reactions. In this work, we have expanded the applicability of commercially available advanced Ni/C, NiMo/C and NiRe/C materials from electrocatalysis to heterogeneous catalysis of CO₂ methanation. Our catalytic testing efforts indicate that the monometallic Ni/C material demonstrates the best CO₂ methanation properties, achieving an excellent CO₂ conversion of 83 % at 400 °C with nearly complete selectivity to CH₄ of 99.7 %, plus exhibiting intact performance during 90 h of time-on-stream testing. Such catalytic properties are among the highest reported to date among carbon-supported Ni-based methanation catalysts. Excellent performance of Ni/C stems from the good dispersion of the Ni nanoparticles over N-containing carbon support material.

Original language	English
Pages (from-to)	4770-4779
Number of pages	10
Journal	ChemCatChem
Volume	13
Issue number	22
DOIs	https://doi.org/10.1002/cctc.202101284
State	Published - Nov 22 2021

Funding

L.P.L.G. thanks the Portuguese Foundation for Science and Technology (FCT) for the PhD grant support (SFRH/BD/128986/2017). This work was partially supported by the Associate Laboratory LSRE‐LCM (UIDB/50020/2020) funded by national funds through FCT/MCTES (PIDDAC). O.S.G.P.S. acknowledges FCT funding under the Scientific Employment Stimulus – Institutional Call CEECINST/00049/2018. Yu.V.K. thanks the FCT for support under the CritMag Project (PTDC/NAN‐MAT/28745/2017). Pajarito gratefully acknowledges financial support from US DOE DE‐FE0031878. A.S. gratefully acknowledges financial support from Oak Ridge National Laboratory SEED 10609 project “Single‐Atom Catalysts for CO Conversion”. AS gratefully acknowledgement catalysts samples provided by Pajarito Powder, LLC. 2

Funders	Funder number
Scientific Employment Stimulus	PTDC/NAN‐MAT/28745/2017
U.S. Department of Energy	DE‐FE0031878
Oak Ridge National Laboratory	10609
Fundação para a Ciência e a Tecnologia	SFRH/BD/128986/2017, UIDB/50020/2020
Ministério da Ciência, Tecnologia e Ensino Superior

Keywords

catalyst stability
heterogeneous catalysis
microstructure
nanocatalysts
nickel

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1002/cctc.202101284

Cite this

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title = "New Opportunity for Carbon-Supported Ni-based Electrocatalysts: Gas-Phase CO2 Methanation",

abstract = "The cost-effectiveness and excellent performance of conductive-carbon-supported Ni-based electrocatalysts make them attractive materials for hydrogen oxidation and evolution reactions. However, they were previously unused in gas-phase hydrogenation reactions. In this work, we have expanded the applicability of commercially available advanced Ni/C, NiMo/C and NiRe/C materials from electrocatalysis to heterogeneous catalysis of CO2 methanation. Our catalytic testing efforts indicate that the monometallic Ni/C material demonstrates the best CO2 methanation properties, achieving an excellent CO2 conversion of 83 % at 400 °C with nearly complete selectivity to CH4 of 99.7 %, plus exhibiting intact performance during 90 h of time-on-stream testing. Such catalytic properties are among the highest reported to date among carbon-supported Ni-based methanation catalysts. Excellent performance of Ni/C stems from the good dispersion of the Ni nanoparticles over N-containing carbon support material.",

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author = "Gon{\c c}alves, {Liliana P.L.} and Alexey Serov and Geoffrey McCool and Mikaela Dicome and Sousa, {Juliana P.S.} and Soares, {O. Salom{\'e} G.P.} and Oleksandr Bondarchuk and Petrovykh, {Dmitri Y.} and Lebedev, {Oleg I.} and Pereira, {M. Fernando R.} and Kolen'ko, {Yury V.}",

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AU - Gonçalves, Liliana P.L.

AU - Serov, Alexey

AU - McCool, Geoffrey

AU - Dicome, Mikaela

AU - Sousa, Juliana P.S.

AU - Soares, O. Salomé G.P.

AU - Bondarchuk, Oleksandr

AU - Petrovykh, Dmitri Y.

AU - Lebedev, Oleg I.

AU - Pereira, M. Fernando R.

AU - Kolen'ko, Yury V.

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N2 - The cost-effectiveness and excellent performance of conductive-carbon-supported Ni-based electrocatalysts make them attractive materials for hydrogen oxidation and evolution reactions. However, they were previously unused in gas-phase hydrogenation reactions. In this work, we have expanded the applicability of commercially available advanced Ni/C, NiMo/C and NiRe/C materials from electrocatalysis to heterogeneous catalysis of CO2 methanation. Our catalytic testing efforts indicate that the monometallic Ni/C material demonstrates the best CO2 methanation properties, achieving an excellent CO2 conversion of 83 % at 400 °C with nearly complete selectivity to CH4 of 99.7 %, plus exhibiting intact performance during 90 h of time-on-stream testing. Such catalytic properties are among the highest reported to date among carbon-supported Ni-based methanation catalysts. Excellent performance of Ni/C stems from the good dispersion of the Ni nanoparticles over N-containing carbon support material.

AB - The cost-effectiveness and excellent performance of conductive-carbon-supported Ni-based electrocatalysts make them attractive materials for hydrogen oxidation and evolution reactions. However, they were previously unused in gas-phase hydrogenation reactions. In this work, we have expanded the applicability of commercially available advanced Ni/C, NiMo/C and NiRe/C materials from electrocatalysis to heterogeneous catalysis of CO2 methanation. Our catalytic testing efforts indicate that the monometallic Ni/C material demonstrates the best CO2 methanation properties, achieving an excellent CO2 conversion of 83 % at 400 °C with nearly complete selectivity to CH4 of 99.7 %, plus exhibiting intact performance during 90 h of time-on-stream testing. Such catalytic properties are among the highest reported to date among carbon-supported Ni-based methanation catalysts. Excellent performance of Ni/C stems from the good dispersion of the Ni nanoparticles over N-containing carbon support material.

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