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

IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL
Haoran Jiang , Zhirang Liu , Zichen Wang , Wangbin Zhu , Qiliang Wei , Fei Guo , Wei Chen , Yinghui Jiang , Heng Zhu , Niancai Cheng
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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-CeO2 interface. The well-defined and fully exposed Pt-CeO2 interface was engineered through controlled incorporation of CeO2 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 CeO2 through confinement effects. Importantly, experimental and theoretical analyses reveal that the interaction between CeO2 and Pt NPs strengthens the stability of Pt NPs, modulates the surface charge distribution of Pt, and provides additional adsorbed hydroxyl species (OHads), further boosting the ethanol oxidation capability of Pt. The Pt/CeO2@NPC-300 catalyst not only delivers a maximum mass activity of 1207 mA mgPt−1 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.

Abstract Image

限制氧化铈团簇诱导的界面工程增强了铂纳米粒子的高效乙醇氧化反应
直接乙醇燃料电池(DEFCs)由于其无毒性、低腐蚀性、高能量和功率密度等优点,作为一种有前途的能量转换装置,得到了广泛的研究。然而,开发高效耐用的乙醇氧化反应催化剂仍然是一个重大的挑战。在此,我们通过精确优化Pt- ceo2界面来调节Pt纳米颗粒(NPs)的中间亲和力,以实现高效的EOR性能。通过在氮掺杂多孔碳(NPC)的分层孔结构中控制CeO2纳米团簇的掺入,设计了定义良好且完全暴露的Pt-CeO2界面。NPC的高导电性和丰富的孔隙结构不仅加快了电荷传递速率,而且通过约束效应增强了CeO2的稳定性。重要的是,实验和理论分析表明,CeO2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(OHads),进一步提高了Pt的乙醇氧化能力。Pt/CeO2@NPC-300催化剂不仅提供了1207 mA mgPt−1的最大质量活性,在500次循环后仍保持其初始性能的64.7%,而且具有优异的CO耐磨性。本研究提出了一种创新的催化剂结构设计策略,以促进defc和其他可持续能源技术的发展。
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来源期刊
CiteScore
16.10
自引率
7.10%
发文量
2568
审稿时长
2 months
期刊介绍: The Journal of Colloid and Interface Science publishes original research findings on the fundamental principles of colloid and interface science, as well as innovative applications in various fields. The criteria for publication include impact, quality, novelty, and originality. Emphasis: The journal emphasizes fundamental scientific innovation within the following categories: A.Colloidal Materials and Nanomaterials B.Soft Colloidal and Self-Assembly Systems C.Adsorption, Catalysis, and Electrochemistry D.Interfacial Processes, Capillarity, and Wetting E.Biomaterials and Nanomedicine F.Energy Conversion and Storage, and Environmental Technologies
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