题目: | Composition Engineering of Amorphous Nickel Boride Nanoarchitectures Enabling Highly Efficient Electrosynthesis of Hydrogen Peroxide |
作者: | Jie Wu1,#, Meilin Hou2,#, Ziliang Chen1,3,*, Weiju Hao4, Xuelei Pan5, Hongyuan Yang3, Wanglai Cen5,6, Yang Liu1,*, Hui Huang1, Prashanth W. Menezes3,7,*, and Zhenhui Kang1,* |
单位: | 1Institute of Functional Nano and Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices, Soochow University, Suzhou 215123, P. R. China 2College of Engineering, Hebei Normal University, Shijiazhuang 050024, P. R. China 3Department of Chemistry: Metalorganics and Inorganic Materials, Technische Universität Berlin, Straße des 17 Juni 135, Sekr. C2, 10623 Berlin, Germany 4State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, 430070 P. R. China 5Institute of New Energy and Low Carbon Technology, Sichuan University, Chengdu, 610065 P. R. China 6College of Science, University of Shanghai for Science and Technology, Shanghai, 200093 P. R. China 7Material Chemistry Group for Thin Film Catalysis–CatLab, Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Str. 15, 12489 Berlin, Germany |
Developing advanced electrocatalysts with exceptional two electron (2e−) selectivity, activity, and stability is crucial for driving the oxygen reduction reaction (ORR) to produce hydrogen peroxide (H2O2). Herein, a composition engineering strategy is proposed to flexibly regulate the intrinsic activity of amorphous nickel boride nanoarchitectures for efficient 2e− ORR by oriented reduction of Ni2+ with different amounts of BH4−. Among borides,the amorphous NiB2 delivers the 2e− selectivity close to 99% at 0.4 V and over 93% in a wide potential range, together with a negligible activity decay under prolonged time. Notably, an ultrahigh H2O2 production rate of 4.753 mol gcat−1 h−1 is achieved upon assembling NiB2 in the practical gas diffusion electrode. The combination of X-ray absorption and in situ Raman spectroscopy, as well as transient photovoltage measurements with density functional theory, unequivocally reveal that the atomic ratio between Ni and B induces the local electronic structure diversity, allowing optimization of the adsorption energy of Ni toward *OOH and reducing of the interfacial charge transfer kinetics to preserve the O−O bond. | |
影响因子: | 30.849 |
分区情况: | 一区 |
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责任编辑:郭佳