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DOI	10.1039/d1ee00740h
	Role of oxygen-bound reaction intermediates in selective electrochemical CO2reduction
	Zhi X.; Vasileff A.; Zheng Y.; Jiao Y.; Qiao S.-Z.
发表日期	2021
ISSN	17545692
起始页码	3912
结束页码	3930
卷号	14 期号:7
英文摘要	The electrochemical CO2 reduction reaction (CRR) is intrinsically complex given the multiple possible reaction pathways and end products. Consequently, selectivity is a persistent challenge for the design and operation of CRR electrocatalysts. A detailed understanding of key elementary steps and surface-bound species involved in the C1-C3 pathways is important for directing the reaction to a target product. However, there has been limited success in fully explaining the selectivity of CO2 reduction, such as the competing production of oxygen-free hydrocarbons and oxygen-containing alcohols. Recently, oxygen-bound intermediates have been identified as essential species to help explain the full reaction roadmap for CO2 reduction. This Review explores the important role of oxygen-bound intermediates in affecting CRR selectivity to the many reduction products, ranging from two electron products to higher reduced products. These oxygen-bound intermediates have a big influence on addressing mechanistic aspects of competing reaction pathways, based on extensive analysis of adsorption behaviour, reaction thermodynamics and reaction kinetics. Considering available theoretical calculations, electrochemical measurements and operando spectroscopy observations, we highlight the preferred reaction pathways to certain products when regulated by oxygen-bound species. The geometries of these oxygen-bound intermediates and their binding on a catalyst surface dictate the breakage or preservation of C-O bonds, which has a significant effect on directing selectivity toward a final product. Based on this mechanistic evaluation, we summarize practical techniques for probing the evolution of intermediates and propose possible strategies for promoting the selectivity of electrocatalysts. © The Royal Society of Chemistry.
英文关键词	Carbon dioxide; Catalyst selectivity; Electrocatalysts; Oxygen; Reaction kinetics; Reduction; Thermodynamics; Adsorption behaviour; Design and operations; Electrochemical measurements; Mechanistic aspects; Operando spectroscopy; Reaction thermodynamics; Surface-bound species; Theoretical calculations; Reaction intermediates; carbon dioxide; catalyst; chemical reaction; electrochemical method; oxygen; reduction
语种	英语
来源期刊	Energy & Environmental Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/190620
作者单位	Centre for Materials in Energy and Catalysis (CMEC), School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA 5005, Australia
推荐引用方式 GB/T 7714	Zhi X.,Vasileff A.,Zheng Y.,et al. Role of oxygen-bound reaction intermediates in selective electrochemical CO2reduction[J],2021,14(7).
APA	Zhi X.,Vasileff A.,Zheng Y.,Jiao Y.,&Qiao S.-Z..(2021).Role of oxygen-bound reaction intermediates in selective electrochemical CO2reduction.Energy & Environmental Science,14(7).
MLA	Zhi X.,et al."Role of oxygen-bound reaction intermediates in selective electrochemical CO2reduction".Energy & Environmental Science 14.7(2021).