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对甲醇氧化电催化具有增强的一氧化碳耐受性的铂铜纳米线网络。

Platinum-copper nanowire networks with enhanced CO tolerance toward methanol oxidation electrocatalysis.

作者信息

Xing Shiyue, Liu Zhongliang, Jiang Yingfang, Tang Pinghui, Zhang Jian, Chen Jiatang, Li Huihui, Li Chunzhong

机构信息

Key Laboratory for Ultrafine Materials of Ministry of Education, School of Chemical Engineering, East China University of Science and Technology Shanghai 200237 China

Cornell High Energy Synchrotron Source, Wilson Laboratory, Cornell University Ithaca New York 14853 USA.

出版信息

Chem Sci. 2025 Apr 18. doi: 10.1039/d5sc00656b.

DOI:10.1039/d5sc00656b
PMID:40290339
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12022767/
Abstract

Developing platinum-based electrocatalysts with high CO tolerance for the methanol oxidation reaction (MOR) is crucial for the practical application of direct methanol fuel cells (DMFCs). Herein, we employed a straightforward one-step method to synthesize Pt Cu network nanowires (NWNs), which exhibit the advantages of structural stability and bimetallic ensembles. The synergistic effect of compressive strain and the ligand effect, induced by Cu incorporation, can effectively lower the d-band center of Pt, thereby weakening the adsorption strength of CO on the catalyst surface. The optimized PtCu NWNs deliver a peak mass activity of 1.33 A mg and a specific activity of 4.43 mA cm for the MOR, which are 3.03 and 4.03 times higher than those of commercial Pt/C, respectively. The CO stripping and Fourier transform infrared spectroscopy results indicate their high anti-CO poisoning ability and methanol activation capacity. Moreover, the PtCu NWNs also exhibit an excellent stability with high current densities observed after 3600 s of operation due to the enhanced CO tolerance and the stable three-dimensional (3D) network structure. This work provides a feasible strategy to suppress CO poisoning during the MOR and obtain highly efficient anode catalysts with enhanced durability in the DMFC field.

摘要

开发对甲醇氧化反应(MOR)具有高CO耐受性的铂基电催化剂对于直接甲醇燃料电池(DMFC)的实际应用至关重要。在此,我们采用一种简单的一步法合成了PtCu网络纳米线(NWNs),其具有结构稳定性和双金属组合的优势。由Cu掺入引起的压缩应变和配体效应的协同作用可以有效降低Pt的d带中心,从而削弱CO在催化剂表面的吸附强度。优化后的PtCu NWNs对MOR的峰值质量活性为1.33 A mg,比活性为4.43 mA cm,分别比商业Pt/C高3.03倍和4.03倍。CO脱附及傅里叶变换红外光谱结果表明它们具有高抗CO中毒能力和甲醇活化能力。此外,由于增强的CO耐受性和稳定的三维(3D)网络结构,PtCu NWNs在运行3600 s后也表现出优异的稳定性,具有高电流密度。这项工作为抑制MOR过程中的CO中毒并在DMFC领域获得具有增强耐久性的高效阳极催化剂提供了一种可行的策略。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2f2c/12118128/6bc6f1078423/d5sc00656b-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2f2c/12118128/7715640086ad/d5sc00656b-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2f2c/12118128/aa9652faddfd/d5sc00656b-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2f2c/12118128/0e1a405e24e7/d5sc00656b-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2f2c/12118128/6bc6f1078423/d5sc00656b-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2f2c/12118128/7715640086ad/d5sc00656b-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2f2c/12118128/aa9652faddfd/d5sc00656b-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2f2c/12118128/0e1a405e24e7/d5sc00656b-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2f2c/12118128/6bc6f1078423/d5sc00656b-f4.jpg

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本文引用的文献

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Angew Chem Int Ed Engl. 2024 Oct 1;63(40):e202410413. doi: 10.1002/anie.202410413. Epub 2024 Aug 16.
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Edge-Rich Pt-O-Ce Sites in CeO Supported Patchy Atomic-Layer Pt Enable a Non-CO Pathway for Efficient Methanol Oxidation.CeO负载的片状原子层铂中富含边缘的Pt-O-Ce位点实现了高效甲醇氧化的非CO途径。
Angew Chem Int Ed Engl. 2024 Oct 1;63(40):e202410545. doi: 10.1002/anie.202410545. Epub 2024 Aug 13.
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D-Band Engineering in Pd-Based Nanowire Networks for Further Enhancement in Ethanol Electrooxidation Reaction.
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Small Methods. 2024 Sep;8(9):e2400368. doi: 10.1002/smtd.202400368. Epub 2024 May 15.
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PtPdCuGa Intermetallic Nanocatalysts with Enhanced Methanol Oxidation Performance for Efficient Hybrid Seawater Electrolysis.具有增强甲醇氧化性能的PtPdCuGa金属间化合物纳米催化剂用于高效混合海水电解
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