格式化
过电位
法拉第效率
氧化还原
电催化剂
甲酸
电化学
活动站点
化学
无机化学
催化作用
材料科学
电极
化学工程
物理化学
有机化学
工程类
作者
Le Li,Adnan Ozden,Shuyi Guo,F Pelayo Garcı A de Arquer,Chuanhao Wang,Mingzhe Zhang,Jin Zhang,Haoyang Jiang,Wei Wang,Hao Dong,David Sinton,Edward H. Sargent,Miao Zhong
标识
DOI:10.1038/s41467-021-25573-9
摘要
Abstract Electrochemical reduction of CO 2 (CO 2 R) to formic acid upgrades waste CO 2 ; however, up to now, chemical and structural changes to the electrocatalyst have often led to the deterioration of performance over time. Here, we find that alloying p-block elements with differing electronegativities modulates the redox potential of active sites and stabilizes them throughout extended CO 2 R operation. Active Sn-Bi/SnO 2 surfaces formed in situ on homogeneously alloyed Bi 0.1 Sn crystals stabilize the CO 2 R-to-formate pathway over 2400 h (100 days) of continuous operation at a current density of 100 mA cm −2 . This performance is accompanied by a Faradaic efficiency of 95% and an overpotential of ~ −0.65 V. Operating experimental studies as well as computational investigations show that the stabilized active sites offer near-optimal binding energy to the key formate intermediate *OCHO. Using a cation-exchange membrane electrode assembly device, we demonstrate the stable production of concentrated HCOO – solution (3.4 molar, 15 wt%) over 100 h.
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