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限制在介孔碳空心球中的铂钌原子合金用于加速甲醇氧化。

Pt-Ru atomic alloys confined in mesoporous carbon hollow spheres for accelerating methanol oxidation.

作者信息

Wang Haiyang, Gao Caiyan, Liu Zhongyi, Li Baojun, Dok Kim Young, Feng Jie, Sun Kaihang, Peng Zhikun

机构信息

College of Chemistry, Henan Institute of Advance Technology, College of Ecology and Environment, Zhengzhou University, Zhengzhou 450001, PR China.

School of Resources and Environmental Engineering, Wuhan University of Technology, Wuhan 430070, PR China.

出版信息

J Colloid Interface Sci. 2025 Jan 15;678(Pt B):1004-1011. doi: 10.1016/j.jcis.2024.09.004. Epub 2024 Sep 7.

Abstract

Active and durable electrocatalysts are essential for commercializing direct methanol fuel cells. However, Pt-based catalysts, extensively utilized in the methanol oxidation reaction (MOR), are suffered from resource scarcity and CO poisoning, which degrade MOR activity severely. Herein, PtRu bimetallic catalysts were synthesized by confining PtRu alloys within the shells of mesoporous carbon hollow spheres (MCHS) via a vacuum-assisted impregnation method (PtRu@MCHS). The confinement effect induced by mesoporous carbon hollow spheres resulted in a robust structure of PtRu@MCHS with an ultrafine dispersion of alloy nanoparticles. The experimental and theoretical results confirmed that the boosting electrocatalytic activity and stability of the MOR over PtRu@MCHS were contributed to the regulated electronic structure as well as the superior CO tolerance of atomic Pt site caused by the electronic interaction between single Pt atoms and Ru nanoparticles. This strategy is versatile for the rational design of Pt-based bimetallic catalysts and has a positive impact on MOR performance.

摘要

活性和耐用的电催化剂对于直接甲醇燃料电池的商业化至关重要。然而,在甲醇氧化反应(MOR)中广泛使用的铂基催化剂面临资源稀缺和一氧化碳中毒的问题,这严重降低了MOR活性。在此,通过真空辅助浸渍法将铂钌合金限制在介孔碳空心球(MCHS)的壳层内合成了铂钌双金属催化剂(PtRu@MCHS)。介孔碳空心球引起的限域效应导致PtRu@MCHS具有坚固的结构,合金纳米颗粒超精细分散。实验和理论结果证实,PtRu@MCHS上MOR的电催化活性和稳定性的提高归因于电子结构的调节以及单个铂原子与钌纳米颗粒之间的电子相互作用导致的原子铂位点优异的一氧化碳耐受性。该策略对于合理设计铂基双金属催化剂具有通用性,并且对MOR性能有积极影响。

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