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将多种优势集成于一种催化剂:表面铱调制的铂铁铱锯齿状纳米线上甲醇氧化电催化的非一氧化碳途径

Integration of multiple advantages into one catalyst: non-CO pathway of methanol oxidation electrocatalysis on surface Ir-modulated PtFeIr jagged nanowires.

作者信息

Zhu Rongying, Yu Renqin, Yin Kun, Zhang Shiming, Chung-Yen Jung Joey, Zhao Yufeng, Li Menggang, Xia Zhonghong, Zhang Jiujun

机构信息

Institute for Sustainable Energy, College of Sciences, Shanghai University, Shanghai 200444, China.

School of Materials Science and Engineering, Peking University, Beijing, 100871, China.

出版信息

J Colloid Interface Sci. 2023 Jun 15;640:348-358. doi: 10.1016/j.jcis.2023.02.126. Epub 2023 Feb 28.

DOI:10.1016/j.jcis.2023.02.126
PMID:36867931
Abstract

Developing highly active methanol oxidation electrocatalysts with superior anti-CO poisoning capability remains a grand challenge. Herein, a simple strategy was employed to prepare distinctive PtFeIr jagged nanowires with Ir located at the shell and Pt/Fe located at the core. The PtFeIr jagged nanowire possesses an optimal mass activity of 2.13 A mg and specific activity of 4.25 mA cm, giving the catalyst a great edge over PtFe jagged nanowire (1.63 A mg and 3.75 mA cm) and Pt/C (0.38 A mg and 0.76 mA cm). The in-situ Fourier transform infrared (FTIR) spectroscopy and differential electrochemical mass spectrometry (DEMS) unravel the origin of extraordinary CO tolerance in terms of key reaction intermediates in the non-CO pathway. Density functional theory (DFT) calculations add to the body of evidence that the surface Ir incorporation transforms the selectivity from CO pathway to non-CO pathway. Meanwhile, the presence of Ir serves to optimize surface electronic structure with weakened CO binding strength. We believe this work will advance the understanding of methanol oxidation catalytic mechanism and provide some insight into structural design of efficient electrocatalysts.

摘要

开发具有卓越抗一氧化碳中毒能力的高活性甲醇氧化电催化剂仍然是一项巨大的挑战。在此,我们采用了一种简单的策略来制备独特的PtFeIr锯齿状纳米线,其中Ir位于壳层,Pt/Fe位于核心。PtFeIr锯齿状纳米线具有2.13 A mg的最佳质量活性和4.25 mA cm的比活性,这使得该催化剂相对于PtFe锯齿状纳米线(1.63 A mg和3.75 mA cm)以及Pt/C(0.38 A mg和0.76 mA cm)具有很大优势。原位傅里叶变换红外光谱(FTIR)和差分电化学质谱(DEMS)从非一氧化碳途径中的关键反应中间体角度揭示了其卓越一氧化碳耐受性的起源。密度泛函理论(DFT)计算进一步证明,表面引入Ir将选择性从一氧化碳途径转变为非一氧化碳途径。同时,Ir的存在有助于优化表面电子结构,削弱一氧化碳的结合强度。我们相信这项工作将推动对甲醇氧化催化机理的理解,并为高效电催化剂的结构设计提供一些见解。

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