Tuning the Electron Localization of Gold Enables the Control of Nitrogen‐to‐Ammonia Fixation. Issue 51 (4th November 2019)

• Record Type: Journal Article
• Authors: 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
• Is Part Of: Angewandte Chemie international edition. Volume 58:Issue 51(2019)
• Page Start: 18604
• Page End: 18609
• Publication Date: 2019-11-04
• Subjects: electrocatalysis -- gold -- nanoparticles -- nitrogen reduction reaction -- photoelectrochemistry; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.201909477
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: The (photo)electrochemical N2 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 CoO x layer to tune the local electronic structure of Au nanoparticles with positive valence sites for boosting conversion of N2 to NH3 . The catalysts, possessing high average oxidation states (ca. 40 %), achieve a high NH3 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 N2 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 . Abstract : The fix is N : Tuning the local electronic structure of Au nanoparticles with positive valence sites can boost conversion of N2 to NH3 by controlling N2 adsorption and the concomitant energy barrier of NRR. The introduction of a metal with local electronic structure can offer a new direction for the fabrication of highly efficient catalysts for the N2 reduction reaction (NRR).