Tuning the Electron Localization of Gold Enables the Control of Nitrogen‐to‐Ammonia Fixation
Year: 2019
Type: review
Abstract: 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 .
Institutions: Hunan University, Curtin University, State Key Laboratory of Chemobiosensing and Chemometrics, National Supercomputing Changsha Center, Nanjing Normal University, Jiangsu Collaborative Innovation Center of Biomedical Functional Materials, The University of Queensland, University of the Sunshine Coast, Chinese Academy of Sciences, Shanghai Institute of Ceramics, University of Chinese Academy of Sciences, State Key Laboratory of High Performance Ceramics and Superfine Microstructure
Language: English
Subfield: Catalysis
Field: Chemical Engineering
Domain: Physical Sciences
Open Access status: bronze
Awards: G10337966, G1540052660, G1594674691, 高掺杂度杂原子掺杂石墨烯的可控制备及其电催化氧还原反应性能研究, Smart utilisation of cobaltite based electrodes on solid oxide fuel cells, Coordinated Access to Lightsources to Promote Standards and Optimization, G3994465436, G4593677599, G5028521634, G5380178042, G7003971911, Single-atom catalysts for electrochemical carbon dioxide conversion, A surface characterisation facility, A Digital Mineralogy & Materials Characterisation Hub for Petrology, Mineralogy, Exploration, Metallurgy and Reservoir Characterisation Research
OpenAlex ID: W2974866817