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用于氧还原反应的富含台阶的超薄铂铜地球丰富金属表面

Terrace-Rich Ultrathin PtCu Surface on Earth-Abundant Metal for Oxygen Reduction Reaction.

作者信息

Sun Mingze, Gong Shuyan, Li Zhengwen, Huang Helai, Chen Yanjun, Niu Zhiqiang

机构信息

State Key Laboratory of Chemical Engineering, Department of Chemical Engineering, Tsinghua University, Beijing, 100084, China.

Department of Chemistry Analytical Instrumentation Center, Capital Normal University, Beijing, 100048, China.

出版信息

ACS Nano. 2023 Oct 10;17(19):19421-19430. doi: 10.1021/acsnano.3c07863. Epub 2023 Sep 18.

Abstract

The activity and stability of the platinum electrode toward the oxygen reduction reaction are size-dependent. Although small nanoparticles have high Pt utilization, the undercoordinated Pt sites on their surface are assumed to have too strong oxygen binding strength, thus often leading to compromised activity and surface instability. Herein, we report an extended nanostructured PtCu ultrathin surface to reduce the number of low-coordination sites without sacrificing the electrochemical active surface area (ECSA). The surface shows (111)-oriented characteristics, as proven by electrochemical probe reactions and spectroscopies. The PtCu surface brings over an order of magnitude increase in specific activity relative to commercial Pt/C and nearly 4-fold enhancement in ECSA compared to traditional thin films. Moreover, due to the weak absorption of air impurities (e.g., SO, NO, CO) on highly coordinated sites, the catalyst displays enhanced contaminant tolerance compared with nanoparticulate Pt/C. This work promises a broad screening of extended nanostructured surface catalysts for electrochemical conversions.

摘要

铂电极对氧还原反应的活性和稳定性取决于其尺寸。尽管小纳米颗粒具有较高的铂利用率,但据推测其表面配位不足的铂位点具有过强的氧结合强度,因此常常导致活性受损和表面不稳定。在此,我们报道了一种扩展的纳米结构铂铜超薄表面,以减少低配位位点的数量,同时不牺牲电化学活性表面积(ECSA)。通过电化学探针反应和光谱学证明,该表面呈现(111)取向特征。与商业铂碳相比,铂铜表面的比活性提高了一个数量级以上,与传统薄膜相比,ECSA提高了近4倍。此外,由于空气杂质(如SO、NO、CO)在高配位位点上的吸附较弱,与纳米颗粒铂碳相比,该催化剂表现出更高的污染物耐受性。这项工作有望广泛筛选用于电化学转化的扩展纳米结构表面催化剂。

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