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将PtCo纳米颗粒集成到氮、硫掺杂的多孔碳纳米片上作为用于氧还原和析氢反应的高性能双功能催化剂。

Integrating PtCo nanoparticles on N, S doped pore carbon nanosheets as high-performance bifunctional catalysts for oxygen reduction and hydrogen evolution reactions.

作者信息

Zhou Na, Wang Rui, Liu Kun

机构信息

Key Laboratory of Thermo-Fluid Science and Engineering of Ministry of Education, School of Energy and Power Engineering, Xi'an Jiaotong University, Xi'an, Shaanxi 710049, China.

School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi'an, Shaanxi 710049, China.

出版信息

J Colloid Interface Sci. 2023 Oct 28;654(Pt B):1186-1198. doi: 10.1016/j.jcis.2023.10.143.

Abstract

The development of low-Pt bifunctional electrocatalysts with excellent performance for oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) is critical for the advancement of the hydrogen economy. Here, we have integrated low-loading Pt and Co metals into N, S doped porous carbon nanosheets to obtain composite catalysts encapsulating PtCo alloy nanoparticles (PtCo2@CoS/N-CNS and PtCo2@N-CNS). The acquired PtCo nanoparticles, with dimensions of about 2.5 nm, are uniformly distributed and firmly anchored in N, S doped carbon nanosheets with large specific surface areas and rich pore structure, forming multiple active centers and effectively preventing the aggregation of metal nanoparticles. The PtCo2@CoS/N-CNS and PtCo2@N-CNS display high ORR catalytic mass activity of 1.65 A mg and 1.01 A mg in 0.1 M HClO. The PtCo2@N-CNS catalyst exhibits excellent HER performance in 0.5 M HSO, with a mass activity (at 50 mV) 4.3 times higher than that of Pt/C. The PtCo2@CoS/N-CNS and PtCo2@N-CNS also exhibit stronger ORR and HER stability than Pt/C after accelerated durability tests. The superior catalytic activity performance of catalysts can be attributed to the synergistic effect of multiple active centers of PtCo, CoS and Co-N in the catalysts. The confinement of PtCo nanoparticles by Co metal and N, S doped porous nanosheets derived from graphitic carbon nitride (g-CN) as the template, which can effectively prevent the corrosion and migration of the catalysts under acidic conditions, enhances the catalytic stability of the materials. This study provides a new perspective for the development of economical and efficient bifunctional low-Pt catalysts.

摘要

开发对氧还原反应(ORR)和析氢反应(HER)具有优异性能的低铂双功能电催化剂对氢经济的发展至关重要。在此,我们将低负载的铂和钴金属整合到氮、硫掺杂的多孔碳纳米片中,以获得包裹铂钴合金纳米颗粒的复合催化剂(PtCo2@CoS/N-CNS和PtCo2@N-CNS)。所获得的尺寸约为2.5纳米的铂钴纳米颗粒均匀分布并牢固地锚定在具有大比表面积和丰富孔结构的氮硫掺杂碳纳米片中,形成多个活性中心并有效防止金属纳米颗粒的聚集。PtCo2@CoS/N-CNS和PtCo2@N-CNS在0.1M HClO中显示出1.65 A mg和1.01 A mg的高ORR催化质量活性。PtCo2@N-CNS催化剂在0.5M HSO中表现出优异的HER性能,其质量活性(在50mV时)比Pt/C高4.3倍。经过加速耐久性测试后,PtCo2@CoS/N-CNS和PtCo2@N-CNS还表现出比Pt/C更强的ORR和HER稳定性。催化剂优异的催化活性性能可归因于催化剂中PtCo、CoS和Co-N多个活性中心的协同作用。以石墨相氮化碳(g-CN)为模板的钴金属和氮、硫掺杂多孔纳米片对PtCo纳米颗粒的限制,可有效防止催化剂在酸性条件下的腐蚀和迁移,增强了材料的催化稳定性。本研究为开发经济高效的双功能低铂催化剂提供了新的视角。

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