A Tandem Strategy for Enhancing Electrochemical CO2 Reduction Activity of Single‐Atom Cu‐S1N3 Catalysts via Integration with Cu Nanoclusters. Issue 45 (4th October 2021)

• Record Type: Journal Article
• Authors: Chen, Datong; Zhang, Lu‐Hua; Du, Jian; Wang, Honghai; Guo, Jiangyi; Zhan, Jiayu; Li, Fei; Yu, Fengshou
• Is Part Of: Angewandte Chemie international edition. Volume 60:Issue 45(2021)
• Page Start: 24022
• Page End: 24027
• Publication Date: 2021-10-04
• Subjects: CO production -- Cu clusters -- electrochemical CO2 reduction -- nitrogen and sulfur co-coordination -- tandem strategy; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.202109579
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: We developed a tandem electrocatalyst for CO2 ‐to‐CO conversion comprising the single Cu site co‐coordinated with N and S anchored carbon matrix (Cu‐S1 N3 ) and atomically dispersed Cu clusters (Cu x ), denoted as Cu‐S1 N3 /Cu x . The as‐prepared Cu‐S1 N3 /Cu x composite presents a 100 % Faradaic efficiency towards CO generation (FECO ) at −0.65 V vs. RHE and high FECO over 90 % from −0.55 to −0.75 V, outperforming the analogues with Cu‐N4 (FECO only 54 % at −0.7 V) and Cu‐S1 N3 (FECO 70 % at −0.7 V) configurations. The unsymmetrical Cu‐S1 N3 atomic interface in the carbon basal plane possesses an optimized binding energy for the key intermediate *COOH compared with Cu‐N4 site. At the same time, the adjacent Cu x effectively promotes the protonation of *CO2 − by accelerating water dissociation and offering *H to the Cu‐S1 N3 active sites. This work provides a tandem strategy for facilitating proton‐coupled electron transfer over the atomic‐level catalytic sites. Abstract : A tandem catalyst composed of single Cu sites co‐coordinated with N and S and atomically dispersed Cu clusters (Cu‐S1 N3 /Cu x ) was developed for CO2 ‐to‐CO conversion. The Cu‐S1 N3 /Cu x exhibited a 100 % Faradaic efficiency for CO formation (FECO ), outperforming the single‐atomic Cu‐N4 analogue (FECO =54 %).