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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; Wang, Shuangyin
2019-12-31
Source PublicationANGEWANDTE CHEMIE-INTERNATIONAL EDITION
ISSN1433-7851
SubtypeArticle; Early Access
AbstractThe (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.
Keywordelectrocatalysis gold nanoparticles nitrogen reduction reaction photoelectrochemistry
DOI10.1002/anie.201909477
WOS KeywordREDUCTION REACTION
Language英语
WOS Research AreaChemistry
PublisherWILEY-V C H VERLAG GMBH
Citation statistics
Document Type期刊论文
Identifierhttp://ir.sic.ac.cn/handle/331005/27501
Collection中国科学院上海硅酸盐研究所
Recommended Citation
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).
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