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定制非晶态钯铜纳米结构用于乙醇电氧化中的高效碳-碳键裂解

Tailoring Amorphous PdCu Nanostructures for Efficient C-C Cleavage in Ethanol Electrooxidation.

作者信息

Wang Weicong, Shi Xiatong, He Tianou, Zhang Zhaorui, Yang Xiaolong, Guo Yan-Jun, Chong Ben, Zhang Wen-Min, Jin Mingshang

机构信息

Frontier Institute of Science and Technology, Xi'an Jiaotong University, Xi'an, Shaanxi 710049, China.

State Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Xi'an, Shaanxi 710049, China.

出版信息

Nano Lett. 2022 Sep 14;22(17):7028-7033. doi: 10.1021/acs.nanolett.2c01870. Epub 2022 Jul 20.

Abstract

The large-scale application of direct ethanol fuel cells has long been obstructed by the sluggish ethanol oxidation reaction at the anode. Current wisdom for designing and fabricating EOR electrocatalysts has been focused on crystalline materials, which result in only limited improvement in catalytic efficiency. Here, we report the amorphous PdCu (a-PdCu) nanomaterials as superior EOR electrocatalysts. The amorphization of PdCu catalysts can significantly facilitate the C-C bond cleavage, which thereby affords a C1 path faradic efficiency as high as 69.6%. Further tailoring the size and shape of a-PdCu nanocatalysts through the delicate kinetic control can result in a maximized mass activity up to 15.25 A/mg, outperforming most reported catalysts. Notably, accelerated durability tests indicate that both the isotropic structure and one-dimensional shape can dramatically enhance the catalytic durability of the catalysts. This work provides valuable guidance for the rational design and fabrication of amorphous noble metal-based electrocatalysts for fuel cells.

摘要

长期以来,阳极乙醇氧化反应迟缓一直阻碍着直接乙醇燃料电池的大规模应用。目前,设计和制造乙醇氧化反应(EOR)电催化剂的思路主要集中在晶体材料上,但其催化效率的提高有限。在此,我们报道了非晶态钯铜(a-PdCu)纳米材料作为优异的EOR电催化剂。钯铜催化剂的非晶化能够显著促进碳-碳键的断裂,从而实现高达69.6%的C1路径法拉第效率。通过精细的动力学控制进一步调整a-PdCu纳米催化剂的尺寸和形状,可使质量活性最大化,达到15.25 A/mg,优于大多数已报道的催化剂。值得注意的是,加速耐久性测试表明,各向同性结构和一维形状均可显著提高催化剂的催化耐久性。这项工作为合理设计和制造用于燃料电池的非晶态贵金属基电催化剂提供了有价值的指导。

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