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

Carbon‐supported nitrogen‐coordinated single‐metal site catalysts (i.e., M−N−C, M: Fe, Co, or Ni) are active for the electrochemical CO2 reduction reaction (CO2RR) to CO. Further improving their intrinsic activity and selectivity by tuning their N−M bond structures and coordination is limited. Herei...

Ausführliche Beschreibung

Gespeichert in:
Bibliographische Detailangaben
Veröffentlicht in:Angewandte Chemie (International ed.) Jg. 61; H. 28; S. e202205632 - n/a
Hauptverfasser: 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
Format: Journal Article
Sprache:Englisch
Veröffentlicht: Germany Wiley Subscription Services, Inc 11.07.2022
Wiley
Ausgabe:International ed. in English
Schlagworte:
Carbon dioxide
Catalysts
Catalytic activity
Chemical reduction
CO2 Reduction
Coordination
diatomic metal-nitrogen sites
Dual Metal–Nitrogen Sites
Electrocatalysis
Electrochemistry
ENERGY STORAGE
Iron
M-N-C catalysts
Metals
M−N−C Catalysts
Nickel
Nitrogen
Selectivity
Structural analysis
M-N-C catalysts
electron microscopy
dual metal-nitrogen sites
CO2 reduction
electrocatalysis
ISSN:1433-7851, 1521-3773, 1521-3773
Online-Zugang:Volltext
Tags: Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
Beschreibung
Zusammenfassung:Carbon‐supported nitrogen‐coordinated single‐metal site catalysts (i.e., M−N−C, M: Fe, Co, or Ni) are active for the electrochemical CO2 reduction reaction (CO2RR) to CO. Further improving their intrinsic activity and selectivity by tuning their N−M bond structures and coordination is limited. Herein, we expand the coordination environments of M−N−C catalysts by designing dual‐metal active sites. The Ni‐Fe catalyst exhibited the most efficient CO2RR activity and promising stability compared to other combinations. Advanced structural characterization and theoretical prediction suggest that the most active N‐coordinated dual‐metal site configurations are 2N‐bridged (Fe‐Ni)N6, in which FeN4 and NiN4 moieties are shared with two N atoms. Two metals (i.e., Fe and Ni) in the dual‐metal site likely generate a synergy to enable more optimal *COOH adsorption and *CO desorption than single‐metal sites (FeN4 or NiN4) with improved intrinsic catalytic activity and selectivity. A series of atomically dispersed and nitrogen coordinated dual‐metal sites (e.g., Ni‐Fe, Fe‐Co, and Ni‐Co) was designed. Among all possible dual‐metal site configurations, the predicted 2N‐bridged (Fe‐Ni)N6 sites exhibited the highest CO2RR activity and promising stability. The optimal dual‐metal sites can decrease the energy barriers for the *COOH adsorption (−0.34 eV) and the *CO desorption (0.39 eV), facilitating CO2 reduction to CO.
Bibliographie:These authors contributed equally to this work.
ObjectType-Article-1
SourceType-Scholarly Journals-1
ObjectType-Feature-2
content type line 14
content type line 23
China Scholarship Council
SC0012704; CBET-1804326; 1804534; 201808320253; BK202107; 5197215069; AC05-00OR22725
USDOE Office of Science (SC), Basic Energy Sciences (BES)
National Science Foundation (NSF)
National Natural Science Foundation of China (NSFC)
BNL-223085-2022-JAAM; BNL-223023-2022-JAAM
Natural Science Foundation of Jiangsu Province
ISSN:1433-7851
1521-3773
1521-3773
DOI:10.1002/anie.202205632