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Tuning the Electron Localization of Gold Enables the Control of Nitrogen‐to‐Ammonia Fixation
Author(s) -
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
Publication year - 2019
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201909477
Subject(s) - catalysis , chemistry , ammonia production , redox , electrochemistry , selectivity , reversible hydrogen electrode , valence (chemistry) , ammonia , adsorption , desorption , hydrogen , nitrogen , nanotechnology , inorganic chemistry , electrode , materials science , working electrode , organic chemistry
The (photo)electrochemical N 2 reduction reaction (NRR) provides a favorable avenue for the production of NH 3 using renewable energy in mild operating conditions. Understanding and building an efficient catalyst with high NH 3 selectivity represents an area of intense interest for the early stages of development for NRR. Herein, we introduce a CoO x layer to tune the local electronic structure of Au nanoparticles with positive valence sites for boosting conversion of N 2 to NH 3 . The catalysts, possessing high average oxidation states (ca. 40 %), achieve a high NH 3 yield rate of 15.1 μg 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 NH 3 .