Journal
SCIENCE BULLETIN
Volume 65, Issue 5, Pages 350-358Publisher
ELSEVIER
DOI: 10.1016/j.scib.2019.12.019
Keywords
Core@shell; Electroreduction; Nitrogen fixation; Vacancy engineering; Amorphous
Categories
Funding
- National Key RAMP
- D Program of China [2016YFA0204100, 2017YFA0208200]
- National Natural Science Foundation of China [21571135]
- Young Thousand Talented Program
- Natural Science Foundation of Jiangsu Higher Education Institutions [17KJB150032]
- Project of Scientific and Technologic Infrastructure of Suzhou [SZS201708]
- Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
- Postgraduate Research AMP
- Practice Innovation Program of Jiangsu Province [KYCX19_1896]
- Soochow University
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The design of electrocatalysts with enhanced adsorption and activation of nitrogen (N-2) is critical for boosting the electrochemical N-2 reduction (ENR). Herein, we developed an efficient strategy to facilitate N-2 adsorption and activation for N-2 electroreduction into ammonia (NH3) by vacancy engineering of core@shell structured Au@SnO2 nanoparticles (NPs). We found that the ultrathin amorphous SnO2 shell with enriched oxygen vacancies was conducive to adsorb N-2 as well as promoted the N-2 activation, meanwhile the metallic Au core ensured the good electrical conductivity for accelerating electrons transport during the electrochemical N-2 reduction reaction, synergistically boosting the N-2 electroreduction catalysis. As confirmed by the N-15-labeling and controlled experiments, the core@shell Au@amorphous SnO2 NPs with abundant oxygen vacancies show the best performance for N-2 electroreduction with the NH3 yield rate of 21.9 mu g h(-1) mg(cat)(1), and faradaic efficiency of 15.2% at -0.2 V-RHE, which surpass the Au@crystalline SnO2 NPs, individual Au NPs and all reported Au-based catalysts for ENR. (C) 2019 Science China Press. Published by Elsevier B.V. and Science China Press. All rights reserved.
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