纳米团簇
催化作用
法拉第效率
串联
电催化剂
质子化
离解(化学)
电化学
电子转移
结晶学
Atom(片上系统)
基面
碳纤维
铜
材料科学
双金属片
化学
金属
纳米技术
物理化学
电极
离子
复合数
冶金
有机化学
复合材料
嵌入式系统
生物化学
计算机科学
作者
Datong Chen,Luhua Zhang,Jian Du,Honghai Wang,Jiangyi Guo,Jing Zhan,Fēi Li,Fengshou Yu
标识
DOI:10.1002/anie.202109579
摘要
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 (Cux ), denoted as Cu-S1 N3 /Cux . The as-prepared Cu-S1 N3 /Cux 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 Cux 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.
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