期刊
ACS CATALYSIS
卷 8, 期 9, 页码 8540-8544出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b02311
关键词
multishelled hollow Cr2O3 microspheres; N-2 reduction reaction; NH3 electrosynthesis; ambient conditions; density functional theory calculations
资金
- National Natural Science Foundation of China [21575137]
Electrohydrogenation of N-2 to NH3 is emerging as an environmentally benign strategy to tackle the issues associated with the energy-intensive, CO2-emitting Haber-Bosch process. However, the method is severely challenged by N-2 activation and needs efficient N-2 reduction reaction (NRR) catalysts. Here, we report that multishelled hollow Cr2O3 microspheres (MHCMs), which are synthesized by a facile synthetic route, can serve as efficient and selective non-noble metal electrocatalysts for NRR. In 0.1 M Na2SO4 solution, the MHCMs achieve a high Faradaic efficiency (6.78%) and a large NH3 yield (25.3 mu g h(-1) mg(cat)(-1)) at -0.9 V vs reversible hydrogen electrode. The MHCMs also exhibit high stability during the reaction. Density functional theory calculations suggest that NRR over MHCMs occurs via both distal associative and partially alternative routes.
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