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用于高电流密度析氢反应的稳健异质纳米碳化物的超快自热合成

Ultrafast self-heating synthesis of robust heterogeneous nanocarbides for high current density hydrogen evolution reaction.

作者信息

Li Chenyu, Wang Zhijie, Liu Mingda, Wang Enze, Wang Bolun, Xu Longlong, Jiang Kaili, Fan Shoushan, Sun Yinghui, Li Jia, Liu Kai

机构信息

State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China.

Shenzhen Geim Graphene Center and Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055, China.

出版信息

Nat Commun. 2022 Jun 9;13(1):3338. doi: 10.1038/s41467-022-31077-x.

Abstract

Designing cost-effective and high-efficiency catalysts to electrolyze water is an effective way of producing hydrogen. Practical applications require highly active and stable hydrogen evolution reaction catalysts working at high current densities (≥1000 mA cm). However, it is challenging to simultaneously enhance the catalytic activity and interface stability of these catalysts. Herein, we report a rapid, energy-saving, and self-heating method to synthesize high-efficiency MoC/MoC/carbon nanotube hydrogen evolution reaction catalysts by ultrafast heating and cooling. The experiments and density functional theory calculations reveal that numerous MoC/MoC hetero-interfaces offer abundant active sites with a moderate hydrogen adsorption free energy ΔG (0.02 eV), and strong chemical bonding between the MoC/MoC catalysts and carbon nanotube heater/electrode significantly enhances the mechanical stability owing to instantaneous high temperature. As a result, the MoC/MoC/carbon nanotube catalyst achieves low overpotentials of 233 and 255 mV at 1000 and 1500 mA cm in 1 M KOH, respectively, and the overpotential shows only a slight change after working at 1000 mA cm for 14 days, suggesting the excellent activity and stability of the high-current-density hydrogen evolution reaction catalyst. The promising activity, excellent stability, and high productivity of our catalyst can fulfil the demands of hydrogen production in various applications.

摘要

设计具有成本效益和高效的水电解催化剂是制氢的有效途径。实际应用需要在高电流密度(≥1000 mA cm)下工作的高活性和稳定的析氢反应催化剂。然而,同时提高这些催化剂的催化活性和界面稳定性具有挑战性。在此,我们报道了一种快速、节能且自热的方法,通过超快加热和冷却来合成高效的MoC/MoC/碳纳米管析氢反应催化剂。实验和密度泛函理论计算表明,大量的MoC/MoC异质界面提供了丰富的活性位点,其氢吸附自由能ΔG适中(0.02 eV),并且MoC/MoC催化剂与碳纳米管加热器/电极之间的强化学键由于瞬时高温而显著提高了机械稳定性。结果,MoC/MoC/碳纳米管催化剂在1 M KOH中,在1000和1500 mA cm下分别实现了233和255 mV的低过电位,并且在1000 mA cm下工作14天后过电位仅略有变化,这表明该高电流密度析氢反应催化剂具有优异的活性和稳定性。我们催化剂具有的良好活性、出色稳定性和高生产率能够满足各种应用中的制氢需求。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6332/9184596/1ed2b0722adb/41467_2022_31077_Fig1_HTML.jpg

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