Single‐Atom Electrocatalysts from Multivariate Metal–Organic Frameworks for Highly Selective Reduction of CO 2 at Low Pressures
Abstract
Abstract Single‐atom catalysts (SACs) are of great interest because of their ultrahigh activity and selectivity. However, it is difficult to construct model SACs according to a general synthetic method, and therefore, discerning differences in activity of diverse single‐atom catalysts is not straightforward. Herein, a general strategy for synthesis of single‐atom metals implanted in N‐doped carbon (M 1 ‐N‐C; M=Fe, Co, Ni and Cu) has been developed starting from multivariate metal–organic frameworks (MOFs). The M 1 ‐N‐C catalysts, featuring identical chemical environments and supports, provided an ideal platform for differentiating the activity of single‐atom metal species. When employed in electrocatalytic CO 2 reduction, Ni 1 ‐N‐C exhibited a very high CO Faradaic efficiency (FE) up to 96.8 % that far surpassed Fe 1 ‐, Co 1 ‐ and Cu 1 ‐N‐C. Remarkably, the best‐performer, Ni 1 ‐N‐C, even demonstrated excellent CO FE at low CO 2 pressures, thereby representing a promising opportunity for the direct use of dilute CO 2 feedstock.
- Authors:
-
[1]
- Hefei National Laboratory for Physical Sciences at the Microscale CAS Key Laboratory of Soft Matter Chemistry Department of Chemistry University of Science and Technology of China Hefei Anhui 230026 P. R. China
- Department of Power Engineering School of Energy, Power and Mechanical Engineering North China Electric Power University Baoding 071003 P. R. China
- Materials Science Division Argonne National Laboratory Lemont IL 60439 USA
- National Synchrotron Radiation Laboratory University of Science and Technology of China Hefei Anhui 230029 P. R. China
- X-ray Science Division Advanced Photon Source Argonne National Laboratory Lemont IL 60439 USA
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1657285
- Resource Type:
- Publisher's Accepted Manuscript
- Journal Name:
- Angewandte Chemie
- Additional Journal Information:
- Journal Name: Angewandte Chemie Journal Volume: 132 Journal Issue: 46; Journal ID: ISSN 0044-8249
- Publisher:
- Wiley Blackwell (John Wiley & Sons)
- Country of Publication:
- Germany
- Language:
- English
Citation Formats
Jiao, Long, Yang, Weijie, Wan, Gang, Zhang, Rui, Zheng, Xusheng, Zhou, Hua, Yu, Shu‐Hong, and Jiang, Hai‐Long. Single‐Atom Electrocatalysts from Multivariate Metal–Organic Frameworks for Highly Selective Reduction of CO 2 at Low Pressures. Germany: N. p., 2020.
Web. doi:10.1002/ange.202008787.
Jiao, Long, Yang, Weijie, Wan, Gang, Zhang, Rui, Zheng, Xusheng, Zhou, Hua, Yu, Shu‐Hong, & Jiang, Hai‐Long. Single‐Atom Electrocatalysts from Multivariate Metal–Organic Frameworks for Highly Selective Reduction of CO 2 at Low Pressures. Germany. https://doi.org/10.1002/ange.202008787
Jiao, Long, Yang, Weijie, Wan, Gang, Zhang, Rui, Zheng, Xusheng, Zhou, Hua, Yu, Shu‐Hong, and Jiang, Hai‐Long. Mon .
"Single‐Atom Electrocatalysts from Multivariate Metal–Organic Frameworks for Highly Selective Reduction of CO 2 at Low Pressures". Germany. https://doi.org/10.1002/ange.202008787.
@article{osti_1657285,
title = {Single‐Atom Electrocatalysts from Multivariate Metal–Organic Frameworks for Highly Selective Reduction of CO 2 at Low Pressures},
author = {Jiao, Long and Yang, Weijie and Wan, Gang and Zhang, Rui and Zheng, Xusheng and Zhou, Hua and Yu, Shu‐Hong and Jiang, Hai‐Long},
abstractNote = {Abstract Single‐atom catalysts (SACs) are of great interest because of their ultrahigh activity and selectivity. However, it is difficult to construct model SACs according to a general synthetic method, and therefore, discerning differences in activity of diverse single‐atom catalysts is not straightforward. Herein, a general strategy for synthesis of single‐atom metals implanted in N‐doped carbon (M 1 ‐N‐C; M=Fe, Co, Ni and Cu) has been developed starting from multivariate metal–organic frameworks (MOFs). The M 1 ‐N‐C catalysts, featuring identical chemical environments and supports, provided an ideal platform for differentiating the activity of single‐atom metal species. When employed in electrocatalytic CO 2 reduction, Ni 1 ‐N‐C exhibited a very high CO Faradaic efficiency (FE) up to 96.8 % that far surpassed Fe 1 ‐, Co 1 ‐ and Cu 1 ‐N‐C. Remarkably, the best‐performer, Ni 1 ‐N‐C, even demonstrated excellent CO FE at low CO 2 pressures, thereby representing a promising opportunity for the direct use of dilute CO 2 feedstock.},
doi = {10.1002/ange.202008787},
journal = {Angewandte Chemie},
number = 46,
volume = 132,
place = {Germany},
year = {Mon Nov 09 00:00:00 EST 2020},
month = {Mon Nov 09 00:00:00 EST 2020}
}
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