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

Angew Chem Int Ed Engl

State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, Hunan, China.

Published: December 2019

The (photo)electrochemical N reduction reaction (NRR) provides a favorable avenue for the production of NH using renewable energy in mild operating conditions. Understanding and building an efficient catalyst with high NH selectivity represents an area of intense interest for the early stages of development for NRR. Herein, we introduce a CoO layer to tune the local electronic structure of Au nanoparticles with positive valence sites for boosting conversion of N to NH . The catalysts, possessing high average oxidation states (ca. 40 %), achieve a high NH yield rate of 15.1 μg cm  h 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 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 .

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http://dx.doi.org/10.1002/anie.201909477DOI Listing

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