Tuning the Electron Localization of Gold Enables the Control of Nitrogen-to-Ammonia Fixation

doi:10.1002/anie.201909477

	Tuning the Electron Localization of Gold Enables the Control of Nitrogen-to-Ammonia Fixation
	Zheng, Jianyun; Lyu, Yanhong; Qiao, Man; Veder, Jean P.; Marco, Roland D.; Bradley, John; Wang, Ruilun; Li, Yafei; Huang, Aibin; Jiang, San Ping
刊名	ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
	2019-12-31
关键词	electrocatalysis gold nanoparticles nitrogen reduction reaction photoelectrochemistry
ISSN号	1433-7851
DOI	10.1002/anie.201909477
文献子类	Article; Early Access
英文摘要	The (photo)electrochemical N-2 reduction reaction (NRR) provides a favorable avenue for the production of NH3 using renewable energy in mild operating conditions. Understanding and building an efficient catalyst with high NH3 selectivity represents an area of intense interest for the early stages of development for NRR. Herein, we introduce a CoOx layer to tune the local electronic structure of Au nanoparticles with positive valence sites for boosting conversion of N-2 to NH3. The catalysts, possessing high average oxidation states (ca. 40 %), achieve a high NH3 yield rate of 15.1 mu g cm(-2) h(-1) and a good faradic efficiency of 19 % at -0.5 V versus reversible hydrogen electrode. Experimental results and simulations reveal that the ability to tune the oxidation state of Au enables the control of N-2 adsorption and the concomitant energy barrier of NRR. Altering the Au oxidation state provides a unique strategy for control of NRR in the production of valuable NH3.
WOS关键词	REDUCTION REACTION
WOS研究方向	Chemistry
语种	英语
出版者	WILEY-V C H VERLAG GMBH
内容类型	期刊论文
源URL	[http://ir.sic.ac.cn/handle/331005/27501]
专题	中国科学院上海硅酸盐研究所
推荐引用方式 GB/T 7714	Zheng, Jianyun,Lyu, Yanhong,Qiao, Man,et al. Tuning the Electron Localization of Gold Enables the Control of Nitrogen-to-Ammonia Fixation[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2019.
APA	Zheng, Jianyun.,Lyu, Yanhong.,Qiao, Man.,Veder, Jean P..,Marco, Roland D..,...&Wang, Shuangyin.(2019).Tuning the Electron Localization of Gold Enables the Control of Nitrogen-to-Ammonia Fixation.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION.
MLA	Zheng, Jianyun,et al."Tuning the Electron Localization of Gold Enables the Control of Nitrogen-to-Ammonia Fixation".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2019).