格式化
催化作用
法拉第效率
循环伏安法
氧化还原
选择性
电化学
吸附
化学
材料科学
化学工程
电流密度
二氧化碳电化学还原
无机化学
物理化学
有机化学
电极
一氧化碳
物理
量子力学
工程类
作者
Haibo Liu,Yunfeng Bai,Meng Wu,Yingchen Yang,Sheng Wang,Jinhui Hao,Longhua Li,Wei‐Cheng Yan,Weidong Shi
标识
DOI:10.1002/anie.202411575
摘要
Renewable electricity shows immense potential as a driving force for the carbon dioxide reduction reaction (CO2RR) in production of formate (HCOO‐) at industrial current density, providing a promising path for value‐added chemicals and chemical manufacturing. However, achieving high selectivity and stable production of HCOO‐ at industrial current density remains a challenge. Here, we present a robust Bi0.6Cu0.4 NSs catalyst capable of regenerating necessary catalytic core (Bi‐O) through cyclic voltammetry (CV) treatment. Notably, at 260 mA cm‐2, faradaic efficiency of HCOO‐ reaches an exceptional selectivity to 99.23%, maintaining above 90% even after 400h, which is longest reaction time reported at industrial current density. Furthermore, in stability test, the catalyst was constructed by CV reconstruction to achieve stable and efficient production of HCOO‐. In 20h reaction test, the catalyst has a rate of HCOO‐ production of 13.24mmol m‐2 s‐1, a HCOO‐ concentration of 1.91mol L‐1, and an energy consumption of 129.80kWh kmol‐1. In‐situ Raman spectroscopy reveals the formation of Bi‐O structure during the gradual transformation of catalyst from Bi0.6Cu0.4 NBs to Bi0.6Cu0.4 NSs. Theoretical studies highlight the pivotal role of Bi‐O structure in modifying the adsorption behavior of reaction intermediates, which further reduces energy barrier for *OCHO conversion in CO2RR.
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