Copper-triggered delocalization of bismuth p-orbital favours high-throughput CO2 electroreduction

催化作用 离域电子 材料科学 电化学 氧化还原 催化循环 纳米技术 化学 电极 组合化学 化学物理 无机化学 物理化学 有机化学 冶金
作者
Bowen Liu,Ying Xie,Xiaolei Wang,Chang Gao,Zhimin Chen,Shaolin Mu,Huiyuan Meng,Zichen Song,Shichao Du,Zhiyu Ren
出处
期刊:Applied Catalysis B-environmental [Elsevier]
卷期号:301: 120781-120781 被引量:45
标识
DOI:10.1016/j.apcatb.2021.120781
摘要

At present, formic acid with the high energy value is the promising product generated by the large-scale renewable electricity-driven CO2 conversion, yet challenges remain in the high-throughput and low-energy production accompanied by the considerable selectivity. Herein, in view of the contribution of electronic modulation to electrocatalytic CO2 reduction reaction (CO2RR) activity of catalysts, the thin BiCu-bimetallic film was designed and built on Cu foam (BiCu/CF) by coupling a facile hydrothermal reaction and an immediate electrochemical transformation. The theoretical evidences demonstrate that Bi p-orbital delocalization triggered by the close-contact metal Cu optimizes reaction pathway of CO2RR, and also favours the orbital hybridization between Bi atom and *OCHO intermediate to form more anti-bonding orbitals, resulting in stabilizing *OCHO intermediate and lowering the thermodynamic barrier of CO2RR. Meanwhile, the electron transferred from catalyst-sites to reaction species also accelerates during CO2RR. Integrating the improved intrinsic activity of Bi catalytic-sites and the superiority of Cu foam in exposing more active sites and the mechanical strength, the BiCu/CF electrode with optimal thickness can acquire satisfactory indicators for industrial application, yielding a record formate current density of 856 mA cm−2, higher than 85% Faradic efficiency, along with a remarkable stability, which outperforms state-of-the-art Bi-based catalysts. This study offers potential avenues of engineering orbital delocalization to rationally construct advanced CO2RR electrodes for the carbon-neutral cycle and utilization.
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