Tandem catalysts CuSe/AuX for increasing local *CO concentration to promote the photocatalytic CO2 reduction to C2H4

Electron Pub Date : 2023-08-17 DOI:10.1002/elt2.3
Yifan Yan, Hongzhi Wang, Xinze Bi, Yuezhu Zhao, Wenhang Wang, Mingbo Wu
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Abstract

It is highly desired yet challenging to strategically steer CO2 reduction reaction (CO2RR) toward ethylene (C2H4) with high activity under visible light irradiation. The key to achieving this goal is increasing the local *CO concentration on the catalyst surface and promoting the C-C coupling progress. Here, we prepare tandem catalysts of CuSe/AuX to realize the photocatalytic reduction of CO2 to C2H4 with high activity. Under light irradiation, the loaded Au NPs are used to activate and transfer CO2 to *CO. The generated *CO intermediate could migrate to the surface of CuSe and cause the C-C coupling process. Moreover, the theoretical calculation results show that the transport process of *CO from Au NPs to CuSe is spontaneous, which plays a critical role in guaranteeing the high concentration of *CO intermediate on the surface of CuSe. This work not only reveals the effect of tandem catalysis on CO2RR to C2 products but also explores the most suitable tandem catalyst to produce C2H4 with high activity by adjusting the loading amounts of Au NPs. Thus, it provides a way to adjust the Cu-based catalyst used in the production of C2 products by photocatalytic CO2RR, which may attract extensive attention in the field.

Abstract Image

串联催化剂CuSe/AuX用于提高局部*CO浓度以促进光催化CO2还原为C2H4
在可见光照射下,战略性地将CO2还原反应(CO2RR)导向具有高活性的乙烯(C2H4)是非常期望但具有挑战性的。实现这一目标的关键是提高催化剂表面的局部*CO浓度并促进C-C偶联进展。在这里,我们制备了CuSe/AuX串联催化剂,以实现高活性的CO2光催化还原为C2H4。在光照射下,负载的Au NPs用于活化CO2并将其转移到*CO。生成的*CO中间体可以迁移到CuSe表面并引起C-C耦合过程。此外,理论计算结果表明,*CO从Au NPs到CuSe的传输过程是自发的,这对保证CuSe表面*CO中间体的高浓度起着关键作用。这项工作不仅揭示了串联催化对CO2RR制备C2产物的影响,而且通过调节Au NPs的负载量,探索了最适合生产高活性C2H4的串联催化剂。因此,它提供了一种通过光催化CO2RR调节用于生产C2产品的Cu基催化剂的方法,这可能会引起该领域的广泛关注。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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