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Efficient CO2 Electroreduction with a Monolayer Bi2WO6 through a Metallic Intermediate Surface State
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-09-24 , DOI: 10.1021/acscatal.1c02495
Shengtang Liu 1 , Chun Wang 2 , Jianghua Wu 3 , Bailin Tian 1 , Yamei Sun 1 , Yang Lv 1 , Zhangyan Mu 1 , Yuxia Sun 1 , Xiaoshan Li 1 , Fangyuan Wang 1 , Yiqi Wang 1 , Lingyu Tang 1 , Peng Wang 3 , Yafei Li 2 , Mengning Ding 1
Affiliation  

Electrocatalytic conversion of carbon dioxide to high-value fuels and chemical feedstocks represents a promising solution toward carbon neutrality. Ongoing efforts have been directed to the development of high-performance, mass production, and cost-efficient catalysts, which, in turn, requires a more precise understanding of the operando details of the catalytic interface and fine control over the reaction pathway. Here, we report that a two-dimensional (2D) monolayer Bi2WO6 with high bismuth exposure demonstrates excellent performance for the electrocatalytic conversion of CO2 to formic acid, including the high Faradic efficiency (FE) over a broad potential range (over 90% from 0.9 to 1.3 V vs RHE, >98% FE at 1.0 V vs RHE) and a high current density over 250 mA/cm2 in a flow cell equipped with a gas diffusion electrode (>97% FE). The distinct reaction pathway observed in the electrocatalytic process, in contrast to the photocatalytic reactions, was investigated by density functional theory. Additionally, the mechanistic investigation further elucidates in operando phase transition to a “metallic intermediate state” on monolayer Bi2WO6 during the electrocatalytic process, providing the experimental evidence to the basis of satisfying performance from all Bi-based catalysts in CO2 reduction.

中文翻译:

通过金属中间表面态使用单层 Bi2WO6 进行有效的 CO2 电还原

将二氧化碳电催化转化为高价值燃料和化学原料是实现碳中和的有前途的解决方案。正在进行的努力致力于开发高性能、大规模生产和具有成本效益的催化剂,这反过来需要更精确地了解催化界面的操作细节和对反应途径的精细控制。在这里,我们报告了具有高铋暴露量的二维 (2D) 单层 Bi 2 WO 6表现出优异的 CO 2电催化转化性能甲酸,包括在广泛的电位范围内的高法拉第效率 (FE)(从 0.9 到 1.3 V vs RHE 超过 90%,在 1.0 V vs RHE 时 >98% FE)和超过 250 mA/cm 2的高电流密度在配备有气体扩散电极 (>97% FE) 的流通池中。与光催化反应相反,在电催化过程中观察到的不同反应途径通过密度泛函理论进行了研究。此外,机理研究进一步阐明了在电催化过程中单层 Bi 2 WO 6上的操作相转变到“金属中间态” ,为所有 Bi 基催化剂在 CO 2中满足性能提供了实验证据。 减少。
更新日期:2021-10-15
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