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用于高效电化学二氧化碳还原的铜锡异质结构的相和结构工程。

Phase and structure engineering of copper tin heterostructures for efficient electrochemical carbon dioxide reduction.

机构信息

College of Chemistry, Chemical Engineering and Materials Science, Soochow University, 215123, Jiangsu, China.

Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials, School of Chemistry and Materials Science, Nanjing Normal University, 210023, Nanjing, China.

出版信息

Nat Commun. 2018 Nov 22;9(1):4933. doi: 10.1038/s41467-018-07419-z.

Abstract

While engineering the phase and structure of electrocatalysts could regulate the performance of many typical electrochemical processes, its importance to the carbon dioxide electroreduction has been largely unexplored. Herein, a series of phase and structure engineered copper-tin dioxide catalysts have been created and thoroughly exploited for the carbon dioxide electroreduction to correlate performance with their unique structures and phases. The copper oxide/hollow tin dioxide heterostructure catalyst exhibits promising performance, which can tune the products from carbon monoxide to formic acid at high faradaic efficiency by simply changing the electrolysis potentials from -0.7 V to -1.0 V. The excellent performance is attributed to the abundant copper/tin dioxide interfaces involved in the copper oxide/hollow tin dioxide heterostructure during the electrochemical process, decreasing the reaction free-energies for the formation of COOH* species. Our work reported herein emphasizes the importance of phase and structure modulating of catalysts for enhancing electrochemical CO reduction and beyond.

摘要

虽然工程化电催化剂的相和结构可以调节许多典型电化学过程的性能,但它对二氧化碳电还原的重要性在很大程度上尚未被探索。在此,我们制备了一系列具有相和结构工程化的铜锡二氧化物催化剂,并对其进行了深入研究,以将其性能与其独特的结构和相联系起来。氧化铜/空心锡二氧化物异质结构催化剂表现出了很有前景的性能,通过简单地将电解电势从-0.7 V 改变到-1.0 V,就可以将产物从一氧化碳调至甲酸,同时保持高法拉第效率。优异的性能归因于在电化学过程中,氧化铜/空心锡二氧化物异质结构中存在丰富的铜/锡二氧化物界面,降低了 COOH* 物种形成的反应自由能。我们在此报告的工作强调了催化剂的相和结构调节对于增强电化学 CO 还原及其他方面的重要性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/66e6/6250663/80d140cca79d/41467_2018_7419_Fig1_HTML.jpg

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