用于高效甲醇氧化的晶相控制 PtSn 金属间纳米线

IF 10.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Siyu Cao, Mengfan Li, Zihan Guo, Li Gong, Yangfan Lu, Wenhua Zhang, Yu Ni, Lei Gao, Chao Ma, Hongwen Huang
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引用次数: 0

摘要

开发高效的铂基甲醇氧化反应(MOR)催化剂对于直接甲醇燃料电池至关重要。纳米材料的相工程为提高其催化性能提供了一种前景广阔的策略,然而在一维纳米线(NWs)中实现相调控仍然是一个巨大的挑战。在此,我们报告了一种简便的一锅法合成晶相调控铂锡金属间纳米线(NWs)的方法,通过调整锡前驱体的用量,实现了面心立方铂锡金属间纳米线(FCC-Pt3Sn INTNWs)和六方紧密堆积铂锡金属间纳米线(HCP-PtSn INTNWs)的晶相调控。值得注意的是,FCC-Pt3Sn INTNWs 表现出较高的质量活性和比活性,分别达到 6.4 A mgPt-1 和 11.8 mA cm-2,超过了同类的 HCP-PtSn INTNWs 和商用 Pt/C 催化剂。经过 10,000 秒的耐久性测试后,FCC-Pt3Sn INTNWs 的质量活性仍保持在 5.6 A mgPt-1,是商用 Pt/C 催化剂的 24.3 倍。MOR 性能的显著提高主要归功于相控结构和 CO 中间产物(CO*)的加速去除。理论计算和 CO 汽提实验证明,FCC-Pt3Sn INTNW 通过减少 CO* 的结合和增强 OH 的吸附,降低了 CO* 转化为 COOH* 的能垒,从而显著提高了 MOR 活性、CO 耐受性和稳定性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Crystal-phase-controlled PtSn intermetallic nanowires for efficient methanol oxidation

Developing highly efficient Pt-based methanol oxidation reaction (MOR) catalysts is pivotal for direct methanol fuel cells. Phase engineering of nanomaterials offers a promising strategy to improve their catalytic performance, yet achieving phase modulation in one-dimensional nanowires (NWs) remains a great challenge. Herein, we report a facile and one-pot synthesis approach for the crystal-phase-controlled Pt-Sn intermetallic nanowires (NWs), realizing the crystal-phases regulation of face-centered cubic Pt3Sn intermetallic NWs (FCC-Pt3Sn INTNWs) and hexagonal close-packed PtSn intermetallic NWs (HCP-PtSn INTNWs) by adjusting the amounts of Sn precursors. Notably, the FCC-Pt3Sn INTNWs exhibit high mass and specific activities of 6.4 A mgPt-1 and 11.8 mA cm-2, respectively, surpassing its counterparts, the HCP-PtSn INTNWs and commercial Pt/C catalysts. After a 10,000 s durability test, the FCC-Pt3Sn INTNWs still maintain a mass activity of 5.6 A mgPt-1, which is 24.3 times higher than that of commercial Pt/C catalyst. This dramatic enhancement of MOR performance is primarily attributed to the phasecontrolled structure and accelerated removal of CO intermediates (CO*). Theoretical calculations and CO stripping experiments demonstrate that the FCC-Pt3Sn INTNWs lower the energy barrier for converting CO* into COOH* by reducing CO* binding and enhancing OH adsorption, thus significantly improving the MOR activity, CO tolerance, and stability.

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来源期刊
Science China Chemistry
Science China Chemistry CHEMISTRY, MULTIDISCIPLINARY-
CiteScore
14.40
自引率
7.30%
发文量
3787
审稿时长
2.2 months
期刊介绍: Science China Chemistry, co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China and published by Science China Press, publishes high-quality original research in both basic and applied chemistry. Indexed by Science Citation Index, it is a premier academic journal in the field. Categories of articles include: Highlights. Brief summaries and scholarly comments on recent research achievements in any field of chemistry. Perspectives. Concise reports on thelatest chemistry trends of interest to scientists worldwide, including discussions of research breakthroughs and interpretations of important science and funding policies. Reviews. In-depth summaries of representative results and achievements of the past 5–10 years in selected topics based on or closely related to the research expertise of the authors, providing a thorough assessment of the significance, current status, and future research directions of the field.
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