Methane Catalytic Pyrolysis by Microwave and Thermal Heating over Carbon Nanotube-Supported Catalysts: Productivity, Kinetics, and Energy Efficiency
Abstract
Methane catalytic pyrolysis, which is the reaction to produce hydrogen and carbon without emitting CO2, represents an approach for decarbonization using natural gas as an energy resource. In this work, the endothermic pyrolysis reaction was carried out under two heating scenarios: convective thermal heating and microwave-driven irradiative heating. The pyrolysis reaction was conducted at 550-600 °C over carbon nanotube-supported Ni-Pd and Ni-Cu catalysts. On both catalysts, an enhanced methane conversion rate was observed under microwave irradiation. The enhanced catalytic activity was hypothetically caused by the presence of free electrons in the carbon atoms within CNT that enabled the CNT support to absorb microwave energy effectively and to be heated efficiently by microwave. The microwave catalytic pyrolysis has shown improvement in kinetics, where the apparent activation energy dropped from 45.5 kJ/mol under conventional convective heating to 24.8 kJ/mol under microwave irradiation. When the methane conversion rate is increased by 37 %, the microwave power consumption only changed by 10.8 %. The research demonstrated the potential of transforming natural gas to clean hydrogen and value-added carbon in a more energy-efficient way. Process simulation and techno-economic analysis showed that potentially hydrogen minimum selling price of about $1 /kg H2 could be achieved.
- Authors:
-
[1];
[1];
[1];
[2];
[3];
[3];
[3];
- West Virginia Univ., Morgantown, WV (United States)
- North Carolina State Univ., Raleigh, NC (United States)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- H Quest Vanguard, Inc., Pittsburgh, PA (United States)
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1967350
- Report Number(s):
- PNNL-SA-171877
Journal ID: ISSN 0888-5885
- Grant/Contract Number:
- AC05-76RL01830; FE0031866
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Industrial and Engineering Chemistry Research
- Additional Journal Information:
- Journal Volume: 61; Journal Issue: 15; Journal ID: ISSN 0888-5885
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Catalysts; Electromagnetic radiation; Hydrocarbons; Hydrogen; Pyrolysis
Citation Formats
Jiang, Changle, Wang, I-Wen, Bai, Xinwei, Balyan, Sonit, Robinson, Brandon, Hu, Jianli, Li, Wenyuan, Deibel, Angela, Liu, Xingbo, Li, Fanxing, Neal, Luke M., Dou, Jian, Jiang, Yuan, Dagle, Robert, Lopez-Ruiz, Juan A., and Skoptsov, George. Methane Catalytic Pyrolysis by Microwave and Thermal Heating over Carbon Nanotube-Supported Catalysts: Productivity, Kinetics, and Energy Efficiency. United States: N. p., 2022.
Web. doi:10.1021/acs.iecr.1c05082.
Jiang, Changle, Wang, I-Wen, Bai, Xinwei, Balyan, Sonit, Robinson, Brandon, Hu, Jianli, Li, Wenyuan, Deibel, Angela, Liu, Xingbo, Li, Fanxing, Neal, Luke M., Dou, Jian, Jiang, Yuan, Dagle, Robert, Lopez-Ruiz, Juan A., & Skoptsov, George. Methane Catalytic Pyrolysis by Microwave and Thermal Heating over Carbon Nanotube-Supported Catalysts: Productivity, Kinetics, and Energy Efficiency. United States. https://doi.org/10.1021/acs.iecr.1c05082
Jiang, Changle, Wang, I-Wen, Bai, Xinwei, Balyan, Sonit, Robinson, Brandon, Hu, Jianli, Li, Wenyuan, Deibel, Angela, Liu, Xingbo, Li, Fanxing, Neal, Luke M., Dou, Jian, Jiang, Yuan, Dagle, Robert, Lopez-Ruiz, Juan A., and Skoptsov, George. Thu .
"Methane Catalytic Pyrolysis by Microwave and Thermal Heating over Carbon Nanotube-Supported Catalysts: Productivity, Kinetics, and Energy Efficiency". United States. https://doi.org/10.1021/acs.iecr.1c05082. https://www.osti.gov/servlets/purl/1967350.
@article{osti_1967350,
title = {Methane Catalytic Pyrolysis by Microwave and Thermal Heating over Carbon Nanotube-Supported Catalysts: Productivity, Kinetics, and Energy Efficiency},
author = {Jiang, Changle and Wang, I-Wen and Bai, Xinwei and Balyan, Sonit and Robinson, Brandon and Hu, Jianli and Li, Wenyuan and Deibel, Angela and Liu, Xingbo and Li, Fanxing and Neal, Luke M. and Dou, Jian and Jiang, Yuan and Dagle, Robert and Lopez-Ruiz, Juan A. and Skoptsov, George},
abstractNote = {Methane catalytic pyrolysis, which is the reaction to produce hydrogen and carbon without emitting CO2, represents an approach for decarbonization using natural gas as an energy resource. In this work, the endothermic pyrolysis reaction was carried out under two heating scenarios: convective thermal heating and microwave-driven irradiative heating. The pyrolysis reaction was conducted at 550-600 °C over carbon nanotube-supported Ni-Pd and Ni-Cu catalysts. On both catalysts, an enhanced methane conversion rate was observed under microwave irradiation. The enhanced catalytic activity was hypothetically caused by the presence of free electrons in the carbon atoms within CNT that enabled the CNT support to absorb microwave energy effectively and to be heated efficiently by microwave. The microwave catalytic pyrolysis has shown improvement in kinetics, where the apparent activation energy dropped from 45.5 kJ/mol under conventional convective heating to 24.8 kJ/mol under microwave irradiation. When the methane conversion rate is increased by 37 %, the microwave power consumption only changed by 10.8 %. The research demonstrated the potential of transforming natural gas to clean hydrogen and value-added carbon in a more energy-efficient way. Process simulation and techno-economic analysis showed that potentially hydrogen minimum selling price of about $1 /kg H2 could be achieved.},
doi = {10.1021/acs.iecr.1c05082},
journal = {Industrial and Engineering Chemistry Research},
number = 15,
volume = 61,
place = {United States},
year = {Thu Apr 07 00:00:00 EDT 2022},
month = {Thu Apr 07 00:00:00 EDT 2022}
}
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