催化作用
电化学
法拉第效率
密度泛函理论
化学
吸附
氧化还原
无机化学
氢
化学工程
材料科学
物理化学
有机化学
电极
计算化学
工程类
作者
Shitao Han,Wei Xia,Shuaiqiang Jia,Jiapeng Jiao,Ting Yao,Xue Dong,Sheng Wang,Jianxin Zhai,Jiahao Yang,Yijun Xie,Xueqing Xing,Haihong Wu,Mingyuan He,Buxing Han
标识
DOI:10.1016/j.cej.2023.147735
摘要
Electrochemical CO2 reduction reaction (CO2RR) using renewable energy to produce valuable multicarbon (C2+) products is a promising approach for carbon emission reduction. In this work, we propose a new strategy to enhance the formation of hydrogen-containing intermediates using the excellent abilities of proton transportation and electronic structure modification of phosphorus (P). To realize this, an in situ electrodeposition method was proposed to prepare P-doped Cu catalysts. It was found that the electrodeposition potential significantly impacts the structure and catalytic performance of P-Cu catalysts. Specifically, the catalyst obtained at − 0.5 V vs. Ag/AgCl exhibited exceptional performance for CO2RR towards C2+ products, achieving a Faradaic efficiency (FE) of ∼ 80.2 % and a partial current density of 40.4 mA cm−2 in an H-type cell. Furthermore, the catalyst demonstrated stability for at least 12 h. Experimental and density functional theory (DFT) studies revealed that the free energy of the hydrogenated process could be significantly reduced by the excellent proton transport ability of P, and the interaction of Cu with the unpaired electrons of carbon could be improved, leading to excellent adsorption ability of Cu for the intermediates and high FE of C2+ products.
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