Atomically Dispersed Dual–Metal Site Catalysts for Enhanced CO2 Reduction: Mechanistic Insight into Active Site Structures

Li, Yi; Shan, Weitao; Zachman, Michael J.; Wang, Maoyu; Hwang, Sooyeon; Tabassum, Hassina; Yang, Juan; Yang, Xiaoxuan; Karakalos, Stavros; Feng, Zhenxing; Wang, Guofeng; Wu, Gang

doi:10.1002/anie.202205632

Atomically Dispersed Dual–Metal Site Catalysts for Enhanced CO₂ Reduction: Mechanistic Insight into Active Site Structures

Journal Article · Mon May 09 00:00:00 EDT 2022 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202205632· OSTI ID:1870391

Li, Yi ^[1]; Shan, Weitao ^[2]; Zachman, Michael J. ^[3]; Wang, Maoyu ^[4]; Hwang, Sooyeon ^[5]; Tabassum, Hassina ^[6]; Yang, Juan ^[7]; Yang, Xiaoxuan ^[6]; Karakalos, Stavros ^[8]; Feng, Zhenxing ^[4]; Wang, Guofeng ^[2]; ^[6]

School of Materials Science and Engineering Jiangsu University Zhenjiang 212013 China; Department of Chemical and Biological Engineering University at Buffalo The State University of New York Buffalo NY 14260 USA
Department of Mechanical Engineering and Materials Science University of Pittsburgh Pittsburgh PA 15261 USA
Center for Nanophase Materials Sciences Oak Ridge National Laboratory Oak Ridge TN 37831 USA
School of Chemical Biological and Environmental Engineering Oregon State University Corvallis OR 97331 USA
Center for Functional Nanomaterials Brookhaven National Laboratory Upton NY 11973 USA
Department of Chemical and Biological Engineering University at Buffalo The State University of New York Buffalo NY 14260 USA
School of Materials Science and Engineering Jiangsu University Zhenjiang 212013 China
Department of Chemical Engineering University of South Carolina Columbia SC 29208 USA

Atomically dispersed and nitrogen-coordinated single-metal sites (MN4 = Fe, Co, or Ni) are recognized as active sites for electrochemical reduction of CO2 (CO2RR) to CO. Although tuning the N-M bond structures and coordination of these sites often allows their intrinsic activity to be improved, achievable performance is constrained by the narrow selection of possible of single-metal site structures. Herein, we expand the possible coordination environments of M-N-C catalyst materials by designing dual-metal (e.g., Ni-Fe, Fe-Co, and Ni-Co) active sites. Among the elemental pairs explored, diatomic Ni-Fe catalysts display the most efficient CO2RR activity, highest CO selectivity, and greatest stability. By combining advanced electron microscopy, X-ray absorption spectroscopy, and density functional theory (DFT) calculations of possible N-coordinated dual-metal site configurations, the most effective structure is determined to be 2N-bridged (Fe-Ni)N6, in which FeN4 and NiN4 moieties are connected with two shared N atoms. Further DFT calculations reveal possible synergies that exist between the metal atoms in dual-metal sites, enabling greater catalytic activity and selectivity than single- metal sites for the critical *COOH adsorption and *CO desorption reaction steps, as well as for competitive hydrogen evolution.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: China Scholarship Council; National Natural Science Foundation of China; Natural Science Foundation of Jiangsu Province; U.S. National Science Foundation; USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; SC0012704

OSTI ID:: 1870391

Alternate ID(s):: OSTI ID: 1867731
OSTI ID: 1873166
OSTI ID: 1881118
OSTI ID: 1901153

Report Number(s):: BNL-223023-2022-JAAM; BNL-223085-2022-JAAM

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 28 Vol. 61; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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