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Modulating electronic structure of CoSe2 by Ni doping for efficient electrocatalyst for hydrogen evolution reaction

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Abstract

Developing robust and efficient non-noble electrocatalysts for the hydrogen evolution reaction (HER) is paramount for sustainably producing hydrogen fuel from electrochemical water splitting. Engineering morphology and chemical composition are significant for fabricating electrocatalysts with superior activity and durability. Herein, novel Ni-doped CoSe2 composites are prepared by a facile one-step hydrothermal method. The optimized 1T-phase Co0.75Ni0.25Se2 shows excellent HER performance, exhibiting overpotential of as low as 172 mV at 10 mA·cm–2 and a small Tafel slope of 32.4 mV·dec–1 in 0.5 mol·L−1 H2SO4 solution, approaching that of commercial Pt/C electrocatalyst (30.7 mV·dec–1). Furthermore, the electrocatalyst possesses superior long-term stability under acidic condition. Physicochemical measurements indicate that the homogeneous nanoparticles morphology, the unique electronic structure, and the 1T-phase are responsible for its superior HER performance. This work comes up with a promising strategy in synthesizing other earth-abundant and low-cost catalysts for industrial applications.

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摘要

开发用于析氢反应(HER)的稳定高效的非贵金属电催化剂对于从电化学水裂解中可持续地生产氢燃料至关重要, 催化剂的形貌和化学组成对其特异性和耐腐蚀性具有重要意义。本文采用一步水热法制备了新型镍掺杂硒化钴杂化催化剂。优化后的1T相样品Co0.75Ni0.25Se2表现出优异的性能, 在电流密度达到10mA·cm-2时仅需低至172 mV的过电位。在0.5 mol·L-1 稀硫酸溶液中, 其塔菲尔斜率约为 32.4 mV·dec-1, 此数值已接近商用Pt/C电催化剂(30.7 mV·dec-1)。此外, 该电催化剂在酸性电解液中具有优异的长效稳定性。测试结果表明, 纳米颗粒的均匀形貌、独特的电子结构和1T相是其优异性能的主要原因。本文提出的高效、廉价催化剂合成方法有望在工业中应用于其它非贵金属催化剂。

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 52002254 and 51773049), the National Program for Support of Top-notch Young Professionals, China Aerospace Science and Technology Corporation-Harbin Institute of Technology Joint Center for Technology Innovation Fund (No. HIT15-1A01), Shanghai Academy of Spaceflight Technology Fund (No. SAST2017-126), the Scientific and Technological Cooperation and Development Fund (No. 2017KJHZ002), Sichuan Science and Technology Program (No. 2020YJ0262), Chunhui Plan of Ministry of Education of China, Fundamental Research Funds for the Central Universities, China (No. YJ201893), and State Key Laboratory of Advanced Metals and Materials, China (No. 2019-Z03).

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Authors and Affiliations

  1. School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001, China

    Xiao-Jiao Fang, Li-Ping Ren & Zai-Xing Jiang

  2. College of Materials Science and Engineering, Sichuan University, Chengdu, 610065, China

    Fang Li & Ze-Gao Wang

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  1. Xiao-Jiao Fang
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Fang, XJ., Ren, LP., Li, F. et al. Modulating electronic structure of CoSe2 by Ni doping for efficient electrocatalyst for hydrogen evolution reaction. Rare Met. 41, 901–910 (2022). https://doi.org/10.1007/s12598-021-01819-9

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