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揭示铂基氧还原催化剂脱合金过程中的结构演变

Uncovering Structural Evolution during the Dealloying Process in Pt-Based Oxygen-Reduction Catalyst.

作者信息

Zhang Huijuan, Tan Minyuan, Hu Longfei, Gui Renjie, Liu Xiaokang, Zhang Xue, Sun Zhiguo, Cao Linlin, Yao Tao

机构信息

National Synchrotron Radiation Laboratory, School of Nuclear Science and Technology, University of Science and Technology of China, Hefei, 230029, P.R. China.

Key Laboratory of Precision and Intelligent Chemistry, University of Science and Technology of China, Hefei, 230026, China.

出版信息

J Phys Chem Lett. 2024 Mar 21;15(11):3071-3077. doi: 10.1021/acs.jpclett.4c00260. Epub 2024 Mar 11.

Abstract

The comprehensive understanding toward the dealloying process is crucial for designing alloy catalysts employed in the oxygen reduction reaction (ORR). However, the specific leaching procedure and subsequent reconstruction of the dealloyed catalyst still remain unclear. Herein, we employ X-ray absorption fine structure spectroscopy to monitor the dealloying process of a two-dimensional PtTe ordered alloy, known for its enhanced ORR activity. Our findings reveal the unsynchronous evolutions of Pt and Te sites, wherein the Pt component undergoes a structural transformation prior to the complete leaching of Te, leading to the formation of a defect-rich Pt catalyst. This dealloyed catalyst exhibits a significant enhancement in ORR activity, featuring a half-wave potential of 0.90 V versus the reversible hydrogen electrode and a mass activity of 0.62 A mg, outperforming the performance of commercial Pt/C counterpart. This in-depth understanding of the dealloying mechanism enriches our knowledge for the development of high-performance Pt-based alloy catalysts.

摘要

对脱合金过程的全面理解对于设计用于氧还原反应(ORR)的合金催化剂至关重要。然而,脱合金催化剂的具体浸出过程以及随后的重构仍不清楚。在此,我们采用X射线吸收精细结构光谱来监测二维PtTe有序合金的脱合金过程,该合金以其增强的ORR活性而闻名。我们的研究结果揭示了Pt和Te位点的不同步演变,其中Pt组分在Te完全浸出之前经历结构转变,导致形成富含缺陷的Pt催化剂。这种脱合金催化剂的ORR活性显著增强,相对于可逆氢电极的半波电位为0.90 V,质量活性为0.62 A mg,优于商业Pt/C催化剂的性能。对脱合金机理的深入理解丰富了我们开发高性能Pt基合金催化剂的知识。

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