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Realizing the reduction of N2 to NH3 at low temperature and pressure is always the unremitting pursuit of scientists and then electrochemical nitrogen reduction reaction offers an intriguing alternative. Here, we develop a feasible way, gamma irradiation, for constructing defective structure on the surface of WO3 nanosheets, which is clearly observed at the atomic scale by high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM). The abundant oxygen vacancies ensure WO3 nanosheets with a Faradaic efficiency of 23% at -0.3 V vs. RHE. Moreover, we start from the regulation of the surface state to suppress proton availability towards hydrogen evolution reaction (HER) on the active site and thus boost the selectivity of nitrogen reduction.
The authors acknowledge financial support from the National Natural Science Foundation of China (Nos. 11575084 and 51602153), the Natural Science Foundation of Jiangsu Province (No. BK20160795), and the Fundamental Research Funds for the Central Universities (No. NE2018104). The author also thank a project funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD).