Precision tuning of highly efficient Pt-based ternary alloys on nitrogen-doped multi-wall carbon nanotubes for methanol oxidation reaction

IF 14 1区 化学 Q1 CHEMISTRY, APPLIED 能源化学 Pub Date : 2023-09-18 DOI:10.1016/j.jechem.2023.08.051
Xingqun Zheng , Zhengcheng Wang , Qian Zhou , Qingmei Wang , Wei He , Shun Lu
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引用次数: 1

Abstract

The electrochemical methanol oxidation is a crucial reaction in the conversion of renewable energy. To enable the widespread adoption of direct methanol fuel cells (DMFCs), it is essential to create and engineer catalysts that are both highly effective and robust for conducting the methanol oxidation reaction (MOR). In this work, trimetallic PtCoRu electrocatalysts on nitrogen-doped carbon and multi-wall carbon nanotubes (PtCoRu@NC/MWCNTs) were prepared through a two-pot synthetic strategy. The acceleration of CO oxidation to CO2 and the blocking of CO reduction on adjacent Pt active sites were attributed to the crucial role played by cobalt atoms in the as-prepared electrocatalysts. The precise control of Co atoms loading was achieved through precursor stoichiometry. Various physicochemical techniques were employed to analyze the morphology, element composition, and electronic state of the catalyst. Electrochemical investigations and theoretical calculations confirmed that the Pt1Co3Ru1@NC/MWCNTs exhibit excellent electrocatalytic performance and durability for the process of MOR. The enhanced MOR activity can be attributed to the synergistic effect between the multiple elements resulting from precisely controlled Co loading content on surface of the electrocatalyst, which facilitates efficient charge transfer. This interaction between the multiple components also modifies the electronic structures of active sites, thereby promoting the conversion of intermediates and accelerating the MOR process. Thus, achieving precise control over Co loading in PtCoRu@NC/MWCNTs would enable the development of high-performance catalysts for DMFCs.

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氮掺杂多壁碳纳米管上高效pt基三元合金用于甲醇氧化反应的精密调谐
甲醇电化学氧化是可再生能源转化过程中的一个关键反应。为了使直接甲醇燃料电池(dmfc)得到广泛应用,必须创造和设计高效且坚固的催化剂来进行甲醇氧化反应(MOR)。本研究通过两锅合成策略制备了氮掺杂碳和多壁碳纳米管(PtCoRu@NC/MWCNTs)上的三金属PtCoRu电催化剂。钴原子在电催化剂中起着至关重要的作用,加速了CO氧化成CO2,并阻断了CO在相邻Pt活性位点上的还原。通过前驱体化学计量学实现了Co原子负载的精确控制。采用多种物理化学技术对催化剂的形貌、元素组成和电子态进行了分析。电化学研究和理论计算证实了Pt1Co3Ru1@NC/MWCNTs在MOR过程中表现出优异的电催化性能和耐久性。MOR活性的增强可归因于电催化剂表面Co负载含量的精确控制导致多元素之间的协同作用,从而促进了有效的电荷转移。这种多组分之间的相互作用也改变了活性位点的电子结构,从而促进了中间体的转化,加速了MOR过程。因此,实现对PtCoRu@NC/MWCNTs中Co负载的精确控制将使dmfc高性能催化剂的开发成为可能。
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23.60
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2875
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