Molten-Salt Electrochemical-Assisted Synthesis of the CeO2-OV@GC Composite-Supported Pt Clusters with a Pt–O–Ce Structure for the Oxygen Reduction Reaction

IF 9.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters Pub Date : 2024-05-28 DOI:10.1021/acs.nanolett.4c01226

Chenming Fan, Shixue Dou, Xiaoqiang Zhan, Shenggang Li, Qiang Wang* and Bing Li*,

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Abstract

Highly active and robust Pt-based electrocatalysts for an oxygen reduction reaction (ORR) are of crucial significance for the development of proton exchange membrane fuel cells (PEMFCs). Herein, the high-loading and well-dispersive Pt clusters on graphitic carbon-supported CeO₂ with abundant oxygen vacancies (Pt_AC/CeO₂-O_V@GC) were successfully fabricated by a molten-salt electrochemical-assisted method. The bonding of Pt with the highly electronegative O induces charge redistribution through the Pt–O–Ce structure, thus reducing the adsorption energies of oxygen-containing species. Such a Pt_AC/CeO₂-O_V@GC electrocatalyst exhibits a greatly enhanced ORR performance with a mass activity of 0.41 ± 0.02 A·mg^–1_Pt at 0.9 V versus a reversible hydrogen electrode, which is 2.7 times the value of a commercial Pt/C catalyst and shows negligible activity decay after 20000 cycles of accelerated degradation tests. It is anticipated that this work will provide enlightening guidance on the controllable synthesis and rational design of high-performance Pt-based electrocatalysts for PEMFCs.

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熔盐电化学辅助合成具有 Pt-O-Ce 结构的 CeO2-OV@GC 复合支撑铂簇（用于氧还原反应）。

用于氧还原反应（ORR）的高活性、高稳定性铂基电催化剂对于质子交换膜燃料电池（PEMFC）的开发具有重要意义。本文采用熔盐电化学辅助方法，在石墨碳支撑的具有丰富氧空位的 CeO2（PtAC/CeO2-OV@GC）上成功制备了高负载、高分散的铂团簇。铂与高电负性 O 的结合促使电荷通过 Pt-O-Ce 结构重新分布，从而降低了含氧物种的吸附能。这种 PtAC/CeO2-OV@GC 电催化剂的 ORR 性能大大提高，与可逆氢电极相比，在 0.9 V 电压下的质量活性为 0.41 ± 0.02 A-mg-1Pt，是商用 Pt/C 催化剂的 2.7 倍，而且在 20000 次加速降解测试后，活性衰减可以忽略不计。预计这项工作将为 PEMFCs 用高性能铂基电催化剂的可控合成和合理设计提供启发性指导。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

期刊介绍： Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.