Activated carbon supported Ni, Fe, and bimetallic NiFe catalysts for COx-free H2 production by microwave methane pyrolysis

Ellison, Candice; Lauterbach, Julia; Smith, Mark W.

doi:10.1016/j.ijhydene.2023.11.150

Title: Activated carbon supported Ni, Fe, and bimetallic NiFe catalysts for CO_x-free H₂ production by microwave methane pyrolysis

Journal Article · 26 November 2023 · International Journal of Hydrogen Energy

DOI: https://doi.org/10.1016/j.ijhydene.2023.11.150 · OSTI ID:2373114

^[1];

^[2]; Smith, Mark W. ^[3]

National Energy Technology Lab. (NETL), Morgantown, WV (United States); US Dept. of Agriculture (USDA), Wyndmoor, PA (United States). ARS-Eastern Regional Research Center
National Energy Technology Lab. (NETL), Morgantown, WV (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Wake Forest Univ., Winston-Salem, NC (United States)
National Energy Technology Lab. (NETL), Morgantown, WV (United States)

The goal of this study was to test the effect of metal-impregnated carbon-based catalysts on the conversion of methane to hydrogen gas and solid carbon using microwave reactor technology. Monometallic and bimetallic catalysts on activated carbon supports (Ni/AC, Fe/AC, Ni-Fe/AC) are compared during methane pyrolysis testing. Catalytic methane pyrolysis was carried out in a microwave reactor at reaction temperatures of 600 °C and 800 °C. For comparison, one of the catalysts (Ni-Fe/AC) was tested in a conventionally heated reactor at 800 °C. The prepared catalysts were characterized by X-ray diffraction (XRD), while post-reaction catalysts were characterized by XRD and SEM. During reaction testing, the monometallic Ni/AC catalyst exhibited the best catalytic activity (CH₄ conversion: 46.0 and H₂ yield: 46.9%) when reacted in the microwave reactor, however, it suffered from rapid deactivation from carbon deposition (carbon yield: 0.39 gC/g catalyst). The bimetallic Ni-Fe/AC catalyst was slightly less active (CH₄ conversion: 36.9 and H₂ yield: 40.5%) but it was more resistant to carbon formation (carbon yield: 0.27 gC/g catalyst) suggesting it may have greater long-term stability. The Ni-Fe/AC catalyst was also the most energy efficient as it required the least microwave power to maintain the 800 °C reaction temperature compared to the other catalysts tested. Methane conversion of the bimetallic Ni-Fe/AC at 800 °C under microwave irradiation was three times the conversion under conventional heating at the same reaction temperature. Finally, this work demonstrates the use of microwave-specific catalysts for catalytic methane pyrolysis in a microwave reactor, and can be used as a foundation for further methane pyrolysis process and catalyst optimization for CO_x-free H₂ production.

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Research Organization:: National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV, and Albany, OR (United States)

Sponsoring Organization:: USDOE Office of Fossil Energy and Carbon Management (FECM)

OSTI ID:: 2373114

Report Number(s):: DOE/NETL--2023/3879

Journal Information:: International Journal of Hydrogen Energy, Journal Name: International Journal of Hydrogen Energy Vol. 55; ISSN 0360-3199

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (28)

Methane Pyrolysis for CO ₂ ‐Free H ₂ Production: A Green Process to Overcome Renewable Energies Unsteadiness Sánchez‐Bastardo, Nuria; Schlögl, Robert; Ruland, Holger Chemie Ingenieur Technik, Vol. 92, Issue 10 https://doi.org/10.1002/cite.202000029	journal	August 2020
Application of ordered mesoporous materials as model supports to study catalyst preparation by impregnation and drying Sietsma, Jelle R. A.; Jos van Dillen, A.; de Jongh, Petra E. Scientific Bases for the Preparation of Heterogeneous Catalysts, 95-102 https://doi.org/10.1016/S0167-2991(06)80895-5	book	September 2006
Catalytic performance and characterization of Ni-Fe catalysts for the steam reforming of tar from biomass pyrolysis to synthesis gas Wang, Lei; Li, Dalin; Koike, Mitsuru Applied Catalysis A: General, Vol. 392, Issue 1-2 https://doi.org/10.1016/j.apcata.2010.11.013	journal	January 2011
Microwave-assisted catalytic methane reforming: A review Nguyen, Hoang M.; Sunarso, Jaka; Li, Claudia Applied Catalysis A: General, Vol. 599 https://doi.org/10.1016/j.apcata.2020.117620	journal	June 2020
Ambient pressure synthesis of ammonia using a microwave reactor Wildfire, Christina; Abdelsayed, Victor; Shekhawat, Dushyant Catalysis Communications, Vol. 115 https://doi.org/10.1016/j.catcom.2018.07.010	journal	September 2018
Microwave-assisted conversion of methane over H-(Fe)-ZSM-5: Evidence for formation of hot metal sites Deng, Yifan; Bai, Xinwei; Abdelsayed, Victor Chemical Engineering Journal, Vol. 420 https://doi.org/10.1016/j.cej.2021.129670	journal	September 2021
A review of microwave-assisted process intensified multiphase reactors Goyal, Himanshu; Chen, Tai-Ying; Chen, Weiqi Chemical Engineering Journal, Vol. 430 https://doi.org/10.1016/j.cej.2021.133183	journal	February 2022
Microwave-associated chemistry in environmental catalysis for air pollution remediation: A review Bao, Chaosheng; Serrano-Lotina, Ana; Niu, Mingshuang Chemical Engineering Journal, Vol. 466 https://doi.org/10.1016/j.cej.2023.142902	journal	June 2023
Microwave–material interaction phenomena: Heating mechanisms, challenges and opportunities in material processing Mishra, Radha Raman; Sharma, Apurbba Kumar Composites Part A: Applied Science and Manufacturing, Vol. 81 https://doi.org/10.1016/j.compositesa.2015.10.035	journal	February 2016
Preparation of bimetallic catalysts Ni-Co and Ni-Fe supported on activated carbon for methane decomposition Wang, Yajie; Zhang, Yun; Zhao, Shun Carbon Resources Conversion, Vol. 3 https://doi.org/10.1016/j.crcon.2020.12.002	journal	January 2020
Comparative evaluation of microwave and conventional gasification of different coal types: Experimental reaction studies Ellison, Candice; Abdelsayed, Victor; Smith, Mark Fuel, Vol. 321 https://doi.org/10.1016/j.fuel.2022.124055	journal	August 2022
Promotion of microwave discharge over carbon catalysts for CO2 reforming of CH4 to syngas Zhang, Fusen; Zhang, Xiaorong; Song, Zhanlong Fuel, Vol. 331 https://doi.org/10.1016/j.fuel.2022.125914	journal	January 2023
Synthesis of carbon-supported nickel catalysts for the dry reforming of CH4 Fidalgo, B.; Zubizarreta, L.; Bermúdez, J. M. Fuel Processing Technology, Vol. 91, Issue 7 https://doi.org/10.1016/j.fuproc.2010.02.011	journal	July 2010
Ni–SiO2 and Ni–Fe–SiO2 catalysts for methane decomposition to prepare hydrogen and carbon filaments Wang, Wenhua; Wang, Heyi; Yang, Yong International Journal of Hydrogen Energy, Vol. 37, Issue 11 https://doi.org/10.1016/j.ijhydene.2012.03.003	journal	June 2012
Preparation of activated carbon supported Fe–Al2O3 catalyst and its application for hydrogen production by catalytic methane decomposition Jin, Lijun; Si, Huanhuan; Zhang, Jianbo International Journal of Hydrogen Energy, Vol. 38, Issue 25 https://doi.org/10.1016/j.ijhydene.2013.06.023	journal	August 2013
Microwave-assisted methane decomposition over pyrolysis residue of sewage sludge for hydrogen production Deng, Wenyi; Su, Yaxin; Liu, Shugang International Journal of Hydrogen Energy, Vol. 39, Issue 17 https://doi.org/10.1016/j.ijhydene.2014.04.033	journal	June 2014
Numerical analysis of microwave assisted thermocatalytic decomposition of methane Gadkari, Siddharth; Fidalgo, Beatriz; Gu, Sai International Journal of Hydrogen Energy, Vol. 42, Issue 7 https://doi.org/10.1016/j.ijhydene.2016.09.126	journal	February 2017
Hydrogen production by methane decomposition using bimetallic Ni–Fe catalysts Tezel, Elif; Figen, Halit Eren; Baykara, Sema Z. International Journal of Hydrogen Energy, Vol. 44, Issue 20 https://doi.org/10.1016/j.ijhydene.2018.12.151	journal	April 2019
Technoeconomic analysis for hydrogen and carbon Co-Production via catalytic pyrolysis of methane Riley, Jarrett; Atallah, Chris; Siriwardane, Ranjani International Journal of Hydrogen Energy, Vol. 46, Issue 39 https://doi.org/10.1016/j.ijhydene.2021.03.151	journal	June 2021
Investigation of methane and ethane pyrolysis with highly active and durable iron-alumina catalyst to produce hydrogen and valuable nano carbons: Continuous fluidized bed tests and reaction rate analysis Siriwardane, Ranjani; Riley, Jarrett; Atallah, Christopher International Journal of Hydrogen Energy, Vol. 48, Issue 38 https://doi.org/10.1016/j.ijhydene.2022.12.268	journal	May 2023
CO2-free hydrogen production via microwave-driven methane pyrolysis Dadsetan, Mehran; Khan, Mohammad Fawaz; Salakhi, Mehdi International Journal of Hydrogen Energy, Vol. 48, Issue 39 https://doi.org/10.1016/j.ijhydene.2022.12.353	journal	May 2023
Literature review of the catalytic pyrolysis of methane for hydrogen and carbon production McConnachie, Mark; Konarova, Muxina; Smart, Simon International Journal of Hydrogen Energy, Vol. 48, Issue 66 https://doi.org/10.1016/j.ijhydene.2023.03.123	journal	August 2023
Catalytic decomposition of methane to produce hydrogen: A review Fan, Zeyu; Weng, Wei; Zhou, Jing Journal of Energy Chemistry, Vol. 58 https://doi.org/10.1016/j.jechem.2020.10.049	journal	July 2021
Preparation and improvement of nickel catalyst supported ordered mesoporous spherical silica for thermocatalytic decomposition of methane mahmoodzade, Eisa; Meshkani, Fereshteh; Rezaei, Mehran Journal of the Energy Institute, Vol. 93, Issue 6 https://doi.org/10.1016/j.joei.2020.08.007	journal	December 2020
Methane Catalytic Pyrolysis by Microwave and Thermal Heating over Carbon Nanotube-Supported Catalysts: Productivity, Kinetics, and Energy Efficiency Jiang, Changle; Wang, I-Wen; Bai, Xinwei Industrial & Engineering Chemistry Research, Vol. 61, Issue 15 https://doi.org/10.1021/acs.iecr.1c05082	journal	April 2022
Designing Local Microwave Heating of Metal Nanoparticles/Metal Oxide Substrate Composites Ano, Taishi; Tsubaki, Shuntaro; Fujii, Satoshi The Journal of Physical Chemistry C, Vol. 125, Issue 43 https://doi.org/10.1021/acs.jpcc.1c06650	journal	October 2021
In situ x-ray diffraction study of graphitic carbon formed during heating and cooling of amorphous-C/Ni bilayers Saenger, K. L.; Tsang, J. C.; Bol, A. A. Applied Physics Letters, Vol. 96, Issue 15 https://doi.org/10.1063/1.3397985	journal	April 2010
NiFe2O4-Coated Activated Carbon Composite as a Cathode Material for Lithium–Sulfur Batteries Cheng, Riguang International Journal of Electrochemical Science https://doi.org/10.20964/2020.03.33	journal	March 2020

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08 HYDROGEN
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Title: Activated carbon supported Ni, Fe, and bimetallic NiFe catalysts for COx-free H2 production by microwave methane pyrolysis

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Title: Activated carbon supported Ni, Fe, and bimetallic NiFe catalysts for CO_x-free H₂ production by microwave methane pyrolysis