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集成掺杂钌电催化剂,具有优异的氢吸附-解吸性能和位于中空管状结构上的活性位点,用于促进高效析氢。

Integrated doped-Ru electrocatalyst with excellent H adsorption-desorption and active site on hollow tubular structures for boosting efficient hydrogen evolution.

作者信息

Yin Yuhao, Zhu Yao, Qian Long, Wang Fei, Yuan Ziyu, Dai Yuting, Zhang Tao, Xue Songlin, Yang Dongya, Qiu Fengxian

机构信息

School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, China.

School of Agricultural Engineering, Jiangsu University, Zhenjiang 212013, China.

出版信息

J Colloid Interface Sci. 2025 Jan;677(Pt B):1005-1013. doi: 10.1016/j.jcis.2024.08.137. Epub 2024 Aug 20.

Abstract

Electrochemical water splitting for hydrogen production is an ideal process for clean energy production. However, highly active and low-cost electrocatalysts are essential and challenging. In this work, a multi-component Cu-based catalyst (Ru-M-C-Cu), synergized with ruthenium (Ru) heteroatom doping, was synthesized via a facile immersion-calcination-immersion method. Based on the cotton biomass substrate, a hollow tubular structure was obtained. By virtue of its distinctive structure and high carbon content, cotton biomass assumed a dual role as a sacrificial template and a reducing agent in the eco-friendly synthesis of electrocatalysts, which was instrumental in the creation of a multi-component system augmented by heteroatom doping. The multi-component system was constructed by in-situ transformation and redox reaction during calcination in an oxygen-free environment. The Ru-M-C-Cu catalyst exhibited a competitive overpotential of 108 mV at a current density of 10 mA cm for alkaline hydrogen evolution reaction (HER). The satisfactory catalytic performance of Ru-M-C-Cu can be attributed to the fact that the Ru-O-Cu catalytic centers enhanced the adsorption and desorption abilities of the Cu-O active sites toward hydrogen. Furthermore, the hollow tubular structure allowed the electrolyte to make full contact with the active sites of the Ru-M-C-Cu catalyst, thus accelerated the HER kinetics. The catalyst showed structural and chemical stability after a 12-hour successive test. Besides, the production cost of Ru-M-C-Cu was significantly reduced by 99.1 % than that of commercial 20 % Pt/C, showing the potential as an alternative catalyst by offering a more accessible and sustainable source. This work provides a new design of sustainable low-budget electrocatalysts with the proposed strategies expected for producing clean and renewable hydrogen energy.

摘要

电化学水分解制氢是一种理想的清洁能源生产工艺。然而,高活性和低成本的电催化剂至关重要且具有挑战性。在本工作中,通过简便的浸渍 - 煅烧 - 浸渍法合成了一种与钌(Ru)杂原子掺杂协同作用的多组分铜基催化剂(Ru - M - C - Cu)。基于棉生物质基底,获得了中空管状结构。凭借其独特的结构和高碳含量,棉生物质在电催化剂的绿色合成中兼具牺牲模板和还原剂的双重作用,这有助于创建一个由杂原子掺杂增强的多组分体系。该多组分体系是在无氧环境下煅烧过程中通过原位转变和氧化还原反应构建而成的。Ru - M - C - Cu催化剂在碱性析氢反应(HER)中,电流密度为10 mA cm时表现出108 mV的竞争过电位。Ru - M - C - Cu令人满意的催化性能可归因于Ru - O - Cu催化中心增强了Cu - O活性位点对氢的吸附和解吸能力。此外,中空管状结构使电解质能够与Ru - M - C - Cu催化剂的活性位点充分接触,从而加速了HER动力学。经过12小时的连续测试后,该催化剂显示出结构和化学稳定性。此外,Ru - M - C - Cu的生产成本比商业20% Pt/C显著降低了99.1%,通过提供更易获取和可持续的来源展现出作为替代催化剂的潜力。本工作通过所提出的策略为可持续低成本电催化剂提供了一种新设计,有望用于生产清洁和可再生氢能。

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