电催化剂
格式化
氧合物
催化作用
化学
电化学
铜
水溶液
锡
无机化学
双金属片
SN2反应
金属
物理化学
立体化学
电极
有机化学
作者
Zhen‐Hua Zhao,Jia‐Run Huang,Pei‐Qin Liao,Xiao‐Ming Chen
标识
DOI:10.1002/anie.202301767
摘要
The development of efficient electrocatalysts with non-copper metal sites for electrochemical CO2 reduction reactions (eCO2 RR) to hydrocarbons and oxygenates is highly desirable, but still a great challenge. Herein, a stable metal-organic framework (DMA)4 [Sn2 (THO)2 ] (Sn-THO, THO6- = triphenylene-2,3,6,7,10,11-hexakis(olate), DMA = dimethylammonium) with isolated and distorted octahedral SnO62- active sites is reported as an electrocatalyst for eCO2 RR, showing an exceptional performance for eCO2 RR to the CH4 product rather than the common products formate and CO for reported Sn-based catalysts. The partial current density of CH4 reaches a high value of 34.5 mA cm-2 , surpassing most reported copper-based and all non-Cu metal-based catalysts. Our experimental and theoretical results revealed that the isolated SnO62- active site favors the formation of key *OCOH species to produce CH4 and can greatly inhibit the formation of *OCHO and *COOH species to produce *HCOOH and *CO, respectively.
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