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用于高效氧还原的一维富扭结钯铅纳米线的二维模板导向合成

Two-dimensional template-directed synthesis of one-dimensional kink-rich PdPb nanowires for efficient oxygen reduction.

作者信息

Fu Luhong, Liu Kai, Lyu Zixi, Sun Yu, Cai Junlin, Wang Shupeng, Wang Qiuxiang, Xie Shuifen

机构信息

Xiamen Key Laboratory of Optoelectronic Materials and Advanced Manufacturing, Instrumental Analysis Center, College of Materials Science and Engineering, Huaqiao University, Xiamen 361021, China.

Xiamen Key Laboratory of Optoelectronic Materials and Advanced Manufacturing, Instrumental Analysis Center, College of Materials Science and Engineering, Huaqiao University, Xiamen 361021, China; College of Material and Chemical Engineering, Henan University of Urban Construction, Pingdingshan 467036, Henan, China.

出版信息

J Colloid Interface Sci. 2023 Mar 15;634:827-835. doi: 10.1016/j.jcis.2022.12.091. Epub 2022 Dec 20.

Abstract

Developing facile synthetic strategies toward ultrafine one-dimensional (1D) nanowires (NWs) with rich catalytic hot spots is pivotal for exploring effective heterogeneous catalysts. Herein, we demonstrate a two-dimensional (2D) template-directed strategy for synthesizing 1D kink-rich PdPb NWs with abundant grain boundaries to serve as high-efficiency electrocatalysts toward oxygen reduction reaction (ORR). In this one-pot synthesis, ultrathin Pd nanosheets were initially generated, which then served as self-sacrificial 2D nano-templates. A dynamic equilibrium growth was subsequently established on the 2D Pd nanosheets through the center-selected etching of Pd atoms and edge-preferred co-deposition of Pd/Pb atoms. This was followed by the oriented attachment of the generated Pd/Pb alloy nanograins and fragments. Thus, kink-rich PdPb NWs with rich grain boundary defects were obtained in high yield, and these NWs were used as electrocatalytic active catalysts. The surface electronic interaction between Pd and Pb atoms effectively decreased the surface d-band center to weaken the binding of oxygen-containing intermediates toward improved ORR kinetics. Specifically, the kink-rich PdPb NWs/C catalyst delivered outstanding ORR mass activity and specific activity (2.26 A⋅mg and 2.59 mA⋅cm, respectively) in an alkaline solution. These values were respectively 13.3 and 10.8 times those of state-of-the-art commercial Pt/C catalyst. This study provides an innovative strategy for fabricating defect-rich low-dimensional nanocatalysts for efficient energy conversion catalysis.

摘要

开发出针对具有丰富催化热点的超细一维(1D)纳米线(NWs)的简便合成策略,对于探索有效的多相催化剂至关重要。在此,我们展示了一种二维(2D)模板导向策略,用于合成具有丰富晶界的富含扭结的PdPb纳米线,作为氧还原反应(ORR)的高效电催化剂。在这种一锅法合成中,首先生成超薄的Pd纳米片,然后它们用作自牺牲二维纳米模板。随后通过对Pd原子的中心选择性蚀刻和Pd/Pb原子的边缘优先共沉积,在二维Pd纳米片上建立了动态平衡生长。接着是生成的Pd/Pb合金纳米颗粒和碎片的定向附着。因此,高产率地获得了具有丰富晶界缺陷的富含扭结的PdPb纳米线,并且这些纳米线被用作电催化活性催化剂。Pd和Pb原子之间的表面电子相互作用有效地降低了表面d带中心,以减弱含氧中间体的结合,从而改善ORR动力学。具体而言,富含扭结的PdPb NWs/C催化剂在碱性溶液中表现出出色的ORR质量活性和比活性(分别为2.26 A·mg和2.59 mA·cm)。这些值分别是最先进的商业Pt/C催化剂的13.3倍和10.8倍。这项研究为制造用于高效能量转换催化的富含缺陷的低维纳米催化剂提供了一种创新策略。

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