催化作用
电合成
选择性
甲酸
法拉第效率
无机化学
化学
产量(工程)
铋
电催化剂
电化学
材料科学
物理化学
有机化学
电极
冶金
作者
Jihan Zhang,Kun Zhao,Yue-Ming Ma,Weirui Chen,X. Shi,Chenghua Sun,Qianyu Zhang,Junfeng Niu
标识
DOI:10.1002/sstr.202300323
摘要
Electroreduction of CO 2 into formic acid (HCOOH) is of great economical value and potential for industrialization. However, it is still a substantial challenge due to the lack of efficient catalysts with simultaneously high activity, selectivity, and durability. Herein, a single‐atom bismuth loaded on N‐doped hollow carbon sphere (Bi–SA/NHCS) catalyst is reported and its catalytic activity and selectivity are modulated by changing the coordination structure of Bi center. The obtained Bi–SA/NHCS with a Bi–N 3 site exhibits significantly enhanced electrocatalytic activity and selectivity of HCOOH synthesis from CO 2 reduction. The HCOOH production rate achieves 16.2 mmol L −1 h −1 cm −2 at a current density of 20 mA cm −2 , and its Faradaic efficiency remains 100% during a long‐term reaction. The HCOOH production rate normalized by catalyst loading is at a molar level of nearly 1.5 mol h −1 g cat −1 . The production rate and Faradaic efficiency of HCOOH electrosynthesis on Bi–SA/NHCS are significantly boosted as compared with other catalysts reported in the literature. Experimental and density‐functional theory results demonstrate that the boosted activity and selectivity of HCOOH synthesis owe to the electronic structure modulation to the Bi center via threefold coordinated N‐ligands, leading to a proper binding energy of HOCO* intermediates.
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