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用于高效析氢反应的集成PtCo-分级碳基电催化剂

Integrated PtCo-Hierarchical Carbon Matrix Electrocatalyst for Efficient Hydrogen Evolution Reaction.

作者信息

Liu Shuxuan, Cao Wen, Wu Jie, Hu Enlai, Zhang Jing, Gao Xuehui, Chen Zhongwei

机构信息

Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, College of Chemistry and Materials Science, Zhejiang Normal University, Jinhua 321004, China.

Department of Chemical Engineering, University of Waterloo, 200 University Avenue West, Waterloo, Ontario N2L 3G1, Canada.

出版信息

ACS Appl Mater Interfaces. 2024 Jan 10;16(1):520-529. doi: 10.1021/acsami.3c13199. Epub 2023 Dec 27.

Abstract

Pt-based catalysts are regarded as state-of-the-art electrocatalysts for producing clean hydrogen energy; however, their wide application is restricted by their low abundance, high cost, and poor stability. Herein, we report an integrated PtCo-hierarchical carbon matrix electrocatalyst (Pt/Co@NCNTs, PtCo@NCNTs, PtCo@NCNTs, and PtCo@NCNTs) that is developed using a thermally driven Co migration strategy forming alloy nanoparticles to achieve efficient hydrogen evolution reaction (HER). Benefiting from its electronic regulation effect and unique hierarchical hollow structure, the PtCo@NCNTs catalyst loaded with 11.5 wt % Pt exhibits superior catalytic performance and durability for HER compared with commercial 20 wt % Pt/C. Under both alkaline and acidic conditions, PtCo@NCNTs exhibits excellent HER activity with overpotentials of 21 and 45 mV at 10 mA cm, respectively. Density functional theory (DFT) results further verify that the interaction between Pt and Co in PtCo@NCNTs can modulate electronic rearrangement, optimize the d-band center, and accelerate water dissociation and *H desorption, thereby enhancing HER activity.

摘要

基于铂的催化剂被视为用于生产清洁氢能的先进电催化剂;然而,它们的广泛应用受到其低丰度、高成本和差稳定性的限制。在此,我们报道了一种集成的铂钴-分级碳基电催化剂(Pt/Co@NCNTs、PtCo@NCNTs、PtCo@NCNTs和PtCo@NCNTs),它是采用热驱动钴迁移策略开发的,形成合金纳米颗粒以实现高效析氢反应(HER)。受益于其电子调节效应和独特的分级中空结构,负载11.5 wt%铂的PtCo@NCNTs催化剂与商业20 wt% Pt/C相比,在HER方面表现出优异的催化性能和耐久性。在碱性和酸性条件下,PtCo@NCNTs分别在10 mA cm时表现出优异的HER活性,过电位分别为21和45 mV。密度泛函理论(DFT)结果进一步证实,PtCo@NCNTs中铂和钴之间的相互作用可以调节电子重排,优化d带中心,并加速水离解和*H脱附,从而提高HER活性。

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