Atomically Dispersed Transition Metals on Carbon Nanotubes with Ultrahigh Loading for Selective Electrochemical Carbon Dioxide Reduction
Abstract
Single-atom catalysts (SACs) are the smallest entities for catalytic reactions with projected high atomic efficiency, superior activity, and selectivity; however, practical applications of SACs suffer from a very low metal loading of 1–2 wt%. Here, a class of SACs based on atomically dispersed transition metals on nitrogen-doped carbon nanotubes (MSA-N-CNTs, where M = Ni, Co, NiCo, CoFe, and NiPt) is synthesized with an extraordinarily high metal loading, e.g., 20 wt% in the case of NiSA-N-CNTs, using a new multistep pyrolysis process. Among these materials, NiSA-N-CNTs show an excellent selectivity and activity for the electrochemical reduction of CO2 to CO, achieving a turnover frequency (TOF) of 11.7 s-1 at -0.55 V (vs reversible hydrogen electrode (RHE)), two orders of magnitude higher than Ni nanoparticles supported on CNTs.
- Authors:
-
- Curtin Univ., Perth, WA (Australia)
- Australian Synchrotron, Clayton (Australia)
- Univ. of Western Australia, Perth, WA (Australia)
- Chinese Academy of Sciences (CAS), Shenyang (China)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Curtin Univ., Perth, WA (Australia); Univ. of Sunshine Coast, Queensland (Australia); Univ. of Queensland, Brisbane, QLD (Australia)
- Chinese Academy of Sciences (CAS), Shenyang (China); Tsinghua Univ., Shenzhua (China); King Abdulaziz Univ., Jeddah (Saudi Arabia)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)
- Sponsoring Org.:
- Australian Research Council; National Science Foundation (NSF); National Natural Science Foundation of China (NSFC); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
- OSTI Identifier:
- 1846560
- Alternate Identifier(s):
- OSTI ID: 1419993; OSTI ID: 1543459
- Grant/Contract Number:
- AC05-00OR22725; AC02-05CH11231; DP150102044; DP150102025; LE120100026; ACI-1053575; 51521091
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Materials
- Additional Journal Information:
- Journal Volume: 30; Journal Issue: 13; Journal ID: ISSN 0935-9648
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; single-atom catalyst; carbon dioxide reduction; carbon monoxide; transition metals; Chemistry; Science & Technology - Other Topics; Materials Science; Physics
Citation Formats
Cheng, Yi, Zhao, Shiyong, Johannessen, Bernt, Veder, Jean-Pierre, Saunders, Martin, Rowles, Matthew, Cheng, Min, Liu, Chang, Chisholm, Matthew, De Marco, Roland, Cheng, Hui-Ming, Yang, Shize, and Jiang, San Ping. Atomically Dispersed Transition Metals on Carbon Nanotubes with Ultrahigh Loading for Selective Electrochemical Carbon Dioxide Reduction. United States: N. p., 2018.
Web. doi:10.1002/adma.201706287.
Cheng, Yi, Zhao, Shiyong, Johannessen, Bernt, Veder, Jean-Pierre, Saunders, Martin, Rowles, Matthew, Cheng, Min, Liu, Chang, Chisholm, Matthew, De Marco, Roland, Cheng, Hui-Ming, Yang, Shize, & Jiang, San Ping. Atomically Dispersed Transition Metals on Carbon Nanotubes with Ultrahigh Loading for Selective Electrochemical Carbon Dioxide Reduction. United States. https://doi.org/10.1002/adma.201706287
Cheng, Yi, Zhao, Shiyong, Johannessen, Bernt, Veder, Jean-Pierre, Saunders, Martin, Rowles, Matthew, Cheng, Min, Liu, Chang, Chisholm, Matthew, De Marco, Roland, Cheng, Hui-Ming, Yang, Shize, and Jiang, San Ping. Fri .
"Atomically Dispersed Transition Metals on Carbon Nanotubes with Ultrahigh Loading for Selective Electrochemical Carbon Dioxide Reduction". United States. https://doi.org/10.1002/adma.201706287. https://www.osti.gov/servlets/purl/1846560.
@article{osti_1846560,
title = {Atomically Dispersed Transition Metals on Carbon Nanotubes with Ultrahigh Loading for Selective Electrochemical Carbon Dioxide Reduction},
author = {Cheng, Yi and Zhao, Shiyong and Johannessen, Bernt and Veder, Jean-Pierre and Saunders, Martin and Rowles, Matthew and Cheng, Min and Liu, Chang and Chisholm, Matthew and De Marco, Roland and Cheng, Hui-Ming and Yang, Shize and Jiang, San Ping},
abstractNote = {Single-atom catalysts (SACs) are the smallest entities for catalytic reactions with projected high atomic efficiency, superior activity, and selectivity; however, practical applications of SACs suffer from a very low metal loading of 1–2 wt%. Here, a class of SACs based on atomically dispersed transition metals on nitrogen-doped carbon nanotubes (MSA-N-CNTs, where M = Ni, Co, NiCo, CoFe, and NiPt) is synthesized with an extraordinarily high metal loading, e.g., 20 wt% in the case of NiSA-N-CNTs, using a new multistep pyrolysis process. Among these materials, NiSA-N-CNTs show an excellent selectivity and activity for the electrochemical reduction of CO2 to CO, achieving a turnover frequency (TOF) of 11.7 s-1 at -0.55 V (vs reversible hydrogen electrode (RHE)), two orders of magnitude higher than Ni nanoparticles supported on CNTs.},
doi = {10.1002/adma.201706287},
journal = {Advanced Materials},
number = 13,
volume = 30,
place = {United States},
year = {Fri Feb 09 00:00:00 EST 2018},
month = {Fri Feb 09 00:00:00 EST 2018}
}
Web of Science
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Carbon dioxide electroreduction on single-atom nickel decorated carbon membranes with industry compatible current densities
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- Nature Communications, Vol. 11, Issue 1
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