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用于全pH值下高效析氢反应的钌基催化剂氢吸附自由能的优化

Optimization of the Hydrogen-Adsorption Free Energy of Ru-Based Catalysts towards High-Efficiency Hydrogen Evolution Reaction at all pH.

作者信息

Cheng Min, Geng Hongbo, Yang Yang, Zhang Yufei, Li Cheng Chao

机构信息

School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou, 510006, P.R. China.

出版信息

Chemistry. 2019 Jun 26;25(36):8579-8584. doi: 10.1002/chem.201900790. Epub 2019 May 24.

Abstract

The utilization of noble-metal catalysts for the hydrogen evolution reaction (HER) provides an efficient strategy for hydrogen acquisition. However, exploring catalysts with suitable hydrogen binding strength for the HER process is always of great importance, but extremely challenging. In this work, sulfur and phosphor as electron-withdrawing elements were incorporated into carbon nanotube (CNT)-supported Ru catalysts, which were prepared through a facile solution reduction reaction and post thermo treatment. Owing to the suitable electronegativity provided by P and synergistic effects of the carbon nanotubes, the RuP /CNT achieved a high catalytic performance as a HER electrocatalyst. This may result from the modulation effect of the electronic properties and the depressed adsorption free energy of RuP . Electrochemical tests present that the RuP /CNT composite exhibit a small overpotential of 58 mV at 10 mA cm in acidic electrolyte. In a neutral or alkaline environment, the overpotential is 82 and 40 mV, respectively. The RuP /CNT electrode also possesses stable durability for long-time cycling, suggesting its remarkable property as promising all-pH HER catalyst.

摘要

利用贵金属催化剂进行析氢反应(HER)为获取氢气提供了一种有效策略。然而,探索在HER过程中具有合适氢结合强度的催化剂一直至关重要,但极具挑战性。在这项工作中,作为吸电子元素的硫和磷被引入到碳纳米管(CNT)负载的Ru催化剂中,该催化剂通过简便的溶液还原反应和后续热处理制备而成。由于P提供的合适电负性以及碳纳米管的协同效应,RuP/CNT作为HER电催化剂实现了高催化性能。这可能源于RuP电子性质的调制效应和降低的吸附自由能。电化学测试表明,RuP/CNT复合材料在酸性电解质中10 mA cm时具有58 mV的小过电位。在中性或碱性环境中,过电位分别为82和40 mV。RuP/CNT电极在长时间循环中也具有稳定的耐久性,表明其作为有前景的全pH析氢催化剂具有卓越性能。

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