Hydrogen‐Bonded Organic Framework Supporting Atomic Bi−N <sub>2</sub> O <sub>2</sub> Sites for High‐Efficiency Electrocatalytic CO <sub>2</sub> Reduction
Changli Wang, Zunhang Lv, Yarong Liu, Rui Liu, Caiting Sun, Jinming Wang, Liuhua Li, Xiangjian Liu, Xiao Feng, Wenxiu Yang, Wenxiu Yang, Bo Wang
Abstract
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.