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面向小面的SnO@Ni中空纤维实现安培级CO电还原为甲酸盐,单程转化率达85%。

Facet-oriented SnO@Ni hollow fiber enables ampere-level CO electroreduction to formate with 85% single-pass conversion.

作者信息

Wei Yiheng, Song Yanfang, Zhu Chang, Mao Jianing, Chen Aohui, Feng Guanghui, Wu Gangfeng, Liu Xiaohu, Li Shoujie, Li Guihua, Wang Jiangjiang, Dong Xiao, Wei Wei, Chen Wei

机构信息

CAS Key Laboratory of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, China.

University of Chinese Academy of Sciences, Beijing 100049, China.

出版信息

Innovation (Camb). 2025 Feb 22;6(6):100844. doi: 10.1016/j.xinn.2025.100844. eCollection 2025 Jun 2.

Abstract

The electrochemical conversion of CO into liquid fuels is a promising strategy for achieving carbon neutrality. Tin dioxide (SnO) shows a notable ability to electrocatalytically convert CO into formate, though its efficiency is significantly limited by its low catalytic activity. Herein, we construct facet-oriented SnO nanoflowers all standing on a three-dimensional nickel hollow fiber that exhibits superior CO-to-formate electrocatalytic performance. A formate selectivity of 94% and stability of 300 h with a current density of 1.3 A cm at -1.1 V (vs. reversible hydrogen electrode [RHE]) are attained under ambient conditions. Notably, an extremely high CO single-pass conversion rate of 85% is achieved, outperforming prominent catalysts reported in electrocatalysis. The synergetic combination of the unique nanostructures and their advanced spatial configuration is proposed to be responsible for the facet-oriented SnO with a hierarchical structure, providing fully exposed active sites and facilitating mass and charge transfers. Enhanced mass transfer in the hollow fiber electrode verified by electrochemical measurements and well-retained Sn species confirmed by spectroscopy synergistically boost the high CO conversion activity. spectroscopy and theoretical calculation results demonstrate that the SnO(101) facet favors ∗OCHO intermediate formation and ∗HCOOH desorption, leading to high formate selectivity. This study provides a straightforward approach to the precise fabrication of composite hollow fiber electrodes, enabling highly efficient electrocatalytic reactions with gas molecules.

摘要

将CO电化学转化为液体燃料是实现碳中和的一种很有前景的策略。二氧化锡(SnO)表现出将CO电催化转化为甲酸盐的显著能力,不过其效率受到低催化活性的显著限制。在此,我们构建了全部分立于三维镍空心纤维上的面取向SnO纳米花,其展现出卓越的CO到甲酸盐的电催化性能。在环境条件下,在-1.1 V(相对于可逆氢电极[RHE])下实现了94%的甲酸盐选择性和300小时的稳定性,电流密度为1.3 A cm 。值得注意的是,实现了85%的极高的CO单程转化率,优于电催化领域报道的著名催化剂。独特的纳米结构及其先进的空间构型的协同组合被认为是具有分级结构的面取向SnO的原因,其提供了完全暴露的活性位点并促进了质量和电荷转移。通过电化学测量验证的空心纤维电极中增强的传质以及通过光谱证实的良好保留的Sn物种协同提高了高CO转化活性。光谱和理论计算结果表明,SnO(101)面有利于OCHO中间体的形成和HCOOH的脱附,从而导致高甲酸盐选择性。本研究提供了一种直接的方法来精确制造复合空心纤维电极,实现与气体分子的高效电催化反应。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/01b4/12169250/37df9834c720/fx1.jpg

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