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光催化CO转化反应途径的见解

Insight on Reaction Pathways of Photocatalytic CO Conversion.

作者信息

Wang Yiou, Chen Enqi, Tang Junwang

机构信息

Department of Chemical Engineering, University College London, London WC1E 7JE, U.K.

Department of Physics, Ludwig-Maximilians-Universität München, Königinstr. 10, 80539 Munich, Germany.

出版信息

ACS Catal. 2022 Jun 17;12(12):7300-7316. doi: 10.1021/acscatal.2c01012. Epub 2022 Jun 3.

Abstract

Photocatalytic CO conversion to value-added chemicals is a promising solution to mitigate the current energy and environmental issues but is a challenging process. The main obstacles include the inertness of CO molecule, the sluggish multi-electron process, the unfavorable thermodynamics, and the selectivity control to preferable products. Furthermore, the lack of fundamental understanding of the reaction pathways accounts for the very moderate performance in the field. Therefore, in this Perspective, we attempt to discuss the possible reaction mechanisms toward all C and C value-added products, taking into account the experimental evidence and theoretical calculation on the surface adsorption, proton and electron transfer, and products desorption. Finally, the remaining challenges in the field, including mechanistic understanding, reactor design, economic consideration, and potential solutions, are critically discussed by us.

摘要

光催化将一氧化碳转化为高附加值化学品是缓解当前能源和环境问题的一个有前景的解决方案,但却是一个具有挑战性的过程。主要障碍包括一氧化碳分子的惰性、缓慢的多电子过程、不利的热力学以及对优选产物的选择性控制。此外,对反应途径缺乏基本了解导致该领域的性能非常一般。因此,在这篇展望文章中,我们试图讨论生成所有含碳和增值产物的可能反应机制,同时考虑到关于表面吸附、质子和电子转移以及产物解吸的实验证据和理论计算。最后,我们批判性地讨论了该领域仍然存在的挑战,包括机理理解、反应器设计、经济考量以及潜在的解决方案。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f542/9207809/34de597e83ad/cs2c01012_0001.jpg

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