氢
还原(数学)
电催化剂
无机化学
金属有机骨架
氢气储存
化学
电化学
电极
物理化学
有机化学
几何学
数学
吸附
作者
Changli Wang,Zunhang Lv,Yarong Liu,Rui Liu,Caiting Sun,Jinming Wang,Liuhua Li,Xiangjian Liu,Xiao Feng,Wenxiu Yang,Bo Wang
标识
DOI:10.1002/anie.202404015
摘要
Abstract Single atomic catalysts (SACs) offer a superior platform for studying the structure–activity relationships during electrocatalytic CO 2 reduction reaction (CO 2 RR). Yet challenges still exist to obtain well‐defined and novel site configuration owing to the uncertainty of functional framework‐derived SACs through calcination. Herein, a novel Bi−N 2 O 2 site supported on the (1 1 0) plane of hydrogen‐bonded organic framework (HOF) is reported directly for CO 2 RR. In flow cell, the target catalyst Bi1‐HOF maintains a faradaic efficiency (FE) HCOOH of over 90 % at a wide potential window of 1.4 V. The corresponding partial current density ranges from 113.3 to 747.0 mA cm −2 . And, Bi1‐HOF exhibits a long‐term stability of over 30 h under a successive potential‐step test with a current density of 100–400 mA cm −2 . Density function theory (DFT) calculations illustrate that the novel Bi−N 2 O 2 site supported on the (1 1 0) plane of HOF effectively induces the oriented electron transfer from Bi center to CO 2 molecule, reaching an enhanced CO 2 activation and reduction. Besides, this study offers a versatile method to reach series of M−N 2 O 2 sites with regulable metal centers via the same intercalation mechanism, broadening the platform for studying the structure–activity relationships during CO 2 RR.
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