U.S. DOE Ames Laboratory Iowa State University Ames IA 50011 USA
Department of Chemistry University of Virginia Charlottesville VA 22904 USA
Department of Chemistry Iowa State University Ames IA 50011 USA
School of Chemical, Biological and Materials Engineering University of Oklahoma Norman OK 73019 USA
Institute for Catalysis Hokkaido University Hokkaido 001‐0021 Japan
Department of Civil, Environmental, and Construction Engineering Catalysis Cluster for Renewable Energy and Chemical Transformations (REACT) NanoScience Technology Center (NSTC) University of Central Florida Orlando FL 32816 USA
The electrochemical carbon dioxide reduction reaction (CO 2 RR) is a transformative technology to reduce the carbon footprint of modern society. Single‐site catalysts have been demonstrated as promising catalysts for CO 2 RR, but general synthetic methods for catalysts with high surface area and tunable single‐site metal composition still need to be developed to unambiguously investigate the structure–activity relationship crossing various metal sites. Here, a generalized coordination–condensation strategy is reported to prepare single‐atom metal sites on ordered mesoporous carbon (OMC) with high surface areas (average 800 m 2 g ‐1 ). This method is applicable to a broad range of metal sites (Fe, Co, Ni, Cu, Pt, Pd, Ru, and Rh) with loadings up to 4 wt.%. In particular, the CO 2 RR to carbon monoxide (CO) Faradaic efficiency (FE) with Ni single‐site OMC catalyst reaches 95%. This high FE is maintained even under large current density (>140 mA cm ‐2 ) and in a long‐term study (14 h), which suits the urgently needed large‐scale applications. Theoretical calculations suggest that the enhanced activity on single‐atom Ni sites results from balanced binding energies between key intermediates, COOH and CO, for CO 2 RR, as mediated by the coordination sphere.
Luo, Zhicheng, et al. "General Synthetic Strategy to Ordered Mesoporous Carbon Catalysts with Single‐Atom Metal Sites for Electrochemical CO <sub>2</sub> Reduction." Small, vol. 18, no. 16, Mar. 2022. https://doi.org/10.1002/smll.202107799
Luo, Zhicheng, Yin, Zhouyang, Yu, Jiaqi, et al., "General Synthetic Strategy to Ordered Mesoporous Carbon Catalysts with Single‐Atom Metal Sites for Electrochemical CO <sub>2</sub> Reduction," Small 18, no. 16 (2022), https://doi.org/10.1002/smll.202107799
@article{osti_1847005,
author = {Luo, Zhicheng and Yin, Zhouyang and Yu, Jiaqi and Yan, Yu and Hu, Bing and Nie, Renfeng and Kolln, Anna F. and Wu, Xun and Behera, Ranjan K. and Chen, Minda and others},
title = {General Synthetic Strategy to Ordered Mesoporous Carbon Catalysts with Single‐Atom Metal Sites for Electrochemical CO <sub>2</sub> Reduction},
annote = {Abstract The electrochemical carbon dioxide reduction reaction (CO 2 RR) is a transformative technology to reduce the carbon footprint of modern society. Single‐site catalysts have been demonstrated as promising catalysts for CO 2 RR, but general synthetic methods for catalysts with high surface area and tunable single‐site metal composition still need to be developed to unambiguously investigate the structure–activity relationship crossing various metal sites. Here, a generalized coordination–condensation strategy is reported to prepare single‐atom metal sites on ordered mesoporous carbon (OMC) with high surface areas (average 800 m 2 g ‐1 ). This method is applicable to a broad range of metal sites (Fe, Co, Ni, Cu, Pt, Pd, Ru, and Rh) with loadings up to 4 wt.%. In particular, the CO 2 RR to carbon monoxide (CO) Faradaic efficiency (FE) with Ni single‐site OMC catalyst reaches 95%. This high FE is maintained even under large current density (>140 mA cm ‐2 ) and in a long‐term study (14 h), which suits the urgently needed large‐scale applications. Theoretical calculations suggest that the enhanced activity on single‐atom Ni sites results from balanced binding energies between key intermediates, COOH and CO, for CO 2 RR, as mediated by the coordination sphere. },
doi = {10.1002/smll.202107799},
url = {https://www.osti.gov/biblio/1847005},
journal = {Small},
issn = {ISSN 1613-6810},
number = {16},
volume = {18},
place = {Germany},
publisher = {Wiley Blackwell (John Wiley & Sons)},
year = {2022},
month = {03}}