Suppr超能文献

通过钉扎效应和水活化提高镧掺杂二氧化锡上电化学二氧化碳还原为甲酸盐的效率

Boosting Electrochemical CO Reduction to Formate over La-Doped SnO via Pinning Effect and Water Activation.

作者信息

Wang Yanlin, Li Guilin, Feng Jiaqi, Wang Xue, Xue Qizhou, Cheng Aofei, Liu Boyang, Zeng Shaojuan, Wang Min, Zhang Xiangping

机构信息

State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering and Environment, China University of Petroleum (Beijing), Beijing 102249, China.

Beijing Key Laboratory of Ionic Liquids Clean Process, State Key Laboratory of Multiphase Complex Systems, CAS Key Laboratory of Green Process and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China.

出版信息

J Am Chem Soc. 2025 Aug 28. doi: 10.1021/jacs.5c03978.

Abstract

Electrochemical reduction of CO to formate over Sn-based catalysts offers an effective carbon-neutral approach for chemical production and renewable energy storage. However, poor selectivity under high current densities persists, primarily due to the instability of Sn-O active sites and slow water dissociation. In this work, a La-doped SnO catalyst is synthesized for efficient CO conversion to formate. Detailed in situ experimental and theoretical studies reveal that La doping induces a pinning effect that effectively stabilizes the Sn-O structure, decreasing the energy barrier for *OCHO conversion. Meanwhile, La species accelerate water activation to provide *H species, and then the moderate *H coverage promotes formate production. As a result, the La-doped SnO exhibits high formate selectivity over a broad potential window from -0.8 to -1.2 V vs reversible hydrogen electrode (RHE), achieving a formate Faradaic efficiency of up to 93.2% with a partial current density of -315.4 mA cm at -1.0 V vs RHE. This work may provide insights into the pinning effect and encourage more design strategies to explore lanthanide element doping for efficient CO electroreduction catalysts.

摘要

在锡基催化剂上通过电化学将CO还原为甲酸盐,为化学品生产和可再生能源存储提供了一种有效的碳中性方法。然而,在高电流密度下选择性较差的问题仍然存在,这主要是由于Sn-O活性位点的不稳定性和水离解缓慢所致。在这项工作中,合成了一种La掺杂的SnO催化剂用于将CO高效转化为甲酸盐。详细的原位实验和理论研究表明,La掺杂会引起钉扎效应,有效地稳定Sn-O结构,降低OCHO转化的能垒。同时,La物种加速水活化以提供H物种,然后适度的*H覆盖促进甲酸盐的生成。结果,La掺杂的SnO在相对于可逆氢电极(RHE)为-0.8至-1.2 V的宽电位窗口内表现出高甲酸盐选择性,在相对于RHE为-1.0 V时,甲酸盐法拉第效率高达93.2%,部分电流密度为-315.4 mA cm²。这项工作可能为钉扎效应提供见解,并鼓励更多的设计策略来探索用于高效CO电还原催化剂的镧系元素掺杂。

文献检索

告别复杂PubMed语法,用中文像聊天一样搜索,搜遍4000万医学文献。AI智能推荐,让科研检索更轻松。

立即免费搜索

文件翻译

保留排版,准确专业,支持PDF/Word/PPT等文件格式,支持 12+语言互译。

免费翻译文档

深度研究

AI帮你快速写综述,25分钟生成高质量综述,智能提取关键信息,辅助科研写作。

立即免费体验