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受限氧化铈团簇诱导的界面工程增强铂纳米颗粒用于高效乙醇氧化反应

Confined cerium oxide clusters induced interface engineering enhance platinum nanoparticles for efficient ethanol oxidation reaction.

作者信息

Jiang Haoran, Liu Zhirang, Wang Zichen, Zhu Wangbin, Wei Qiliang, Guo Fei, Chen Wei, Jiang Yinghui, Zhu Heng, Cheng Niancai

机构信息

College of Materials Science and Engineering, Fuzhou University, Fuzhou 350108, China.

Institute of Micro/Nano Materials and Devices, Ningbo University of Technology, Ningbo 315211, China.

出版信息

J Colloid Interface Sci. 2025 Dec;699(Pt 2):138254. doi: 10.1016/j.jcis.2025.138254. Epub 2025 Jun 20.

DOI:10.1016/j.jcis.2025.138254
PMID:40578087
Abstract

Direct ethanol fuel cells (DEFCs) have been extensively studied as promising energy conversion devices due to their non-toxicity, low corrosivity, and high energy and power densities. However, developing highly active and durable catalysts for the ethanol oxidation reaction (EOR) at the anode remains a significant challenge. Herein, we modulate the intermediate affinity on Pt nanoparticles (NPs) to achieve highly efficient EOR performance through precise optimization of the Pt-CeO interface. The well-defined and fully exposed Pt-CeO interface was engineered through controlled incorporation of CeO nanoclusters within the hierarchical pore structure of nitrogen-doped porous carbon (NPC). The high electrical conductivity and abundant pore structure of NPC not only accelerate the charge transfer rate but also enhance the stability of CeO through confinement effects. Importantly, experimental and theoretical analyses reveal that the interaction between CeO and Pt NPs strengthens the stability of Pt NPs, modulates the surface charge distribution of Pt, and provides additional adsorbed hydroxyl species (OH), further boosting the ethanol oxidation capability of Pt. The Pt/CeO@NPC-300 catalyst not only delivers a maximum mass activity of 1207 mA mg and retains 64.7 % of its initial performance after 500 cycles, but also exhibits excellent CO tolerance. This study proposes an innovative catalyst structural design strategy to advance the development of DEFCs and other sustainable energy technologies.

摘要

直接乙醇燃料电池(DEFCs)因其无毒、腐蚀性低、能量和功率密度高而作为有前景的能量转换装置受到广泛研究。然而,开发用于阳极乙醇氧化反应(EOR)的高活性和耐用催化剂仍然是一项重大挑战。在此,我们通过精确优化Pt-CeO界面来调节Pt纳米颗粒(NPs)上的中间体亲和力,以实现高效的EOR性能。通过在氮掺杂多孔碳(NPC)的分级孔结构中可控地掺入CeO纳米团簇,设计出了明确且完全暴露的Pt-CeO界面。NPC的高电导率和丰富的孔结构不仅加速了电荷转移速率,还通过限域效应提高了CeO的稳定性。重要的是,实验和理论分析表明,CeO与Pt NPs之间的相互作用增强了Pt NPs的稳定性,调节了Pt的表面电荷分布,并提供了额外的吸附羟基物种(OH),进一步提高了Pt的乙醇氧化能力。Pt/CeO@NPC-300催化剂不仅具有1207 mA mg的最大质量活性,在500次循环后仍保留其初始性能的64.7%,而且还表现出优异的CO耐受性。本研究提出了一种创新的催化剂结构设计策略,以推动DEFCs和其他可持续能源技术的发展。

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