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原子台阶表面调控的 Pd 纳米线用于提升醇氧化活性。

Atom-stepped surface-regulated Pd nanowires for boosting alcohol oxidation activity.

机构信息

Department of Chemistry, City University of Hong Kong, 83 Tat Chee Avenue, Kowloon, Hong Kong Special Administrative Region.

School of Energy and Environment, City University of Hong Kong, 83 Tat Chee Avenue, Kowloon, Hong Kong S.A.R, China.

出版信息

J Colloid Interface Sci. 2023 Sep 15;646:529-537. doi: 10.1016/j.jcis.2023.05.016. Epub 2023 May 9.

Abstract

A highly active surface can endow the electrocatalysts with extraordinary catalytic performances. However, it remains challenging to tailor the atomic packing characteristics and thus the physical and chemical characteristics of the electrocatalysts. Herein, penta-twinned Pd nanowires (NWs) with abundant high-energy atomic steps (i.e., stepped Pd) are synthesized by seeded synthesis on Pd NWs enclosed by (100) facets. Benefiting from the catalytically active atomic steps, such as [n(100) × m(111)] on the surface, the resultant stepped Pd NWs can work as an effective electrocatalyst for the ethanol oxidation reaction (EOR) and ethylene glycol oxidation reaction (EGOR), which are essential anode reactions in direct alcohol fuel cells (DAFCs). Compared with commercial Pd/C, the Pd nanowires bound by (100) facets and atomic steps both display enhanced catalytic activity and stability towards the EOR and EGOR. Importantly, the mass activities of the stepped Pd NWs toward the EOR and EGOR are 6.38 and 7.98 A mg, which are 3.1 and 2.6 times those of Pd NWs enclosed by (100) facets, respectively. Besides, our synthetic strategy also enables the formation of bimetallic Pd-Cu nanowires with abundant atomic steps. This work not only demonstrates a simple yet effective strategy to obtain mono- or bi-metallic nanowires with abundant atomic steps, but also highlights the significant role of atomic steps for boosting the activity of electrocatalysts.

摘要

高活性表面可以赋予电催化剂非凡的催化性能。然而,通过调整原子堆积特性来改变电催化剂的物理和化学性质仍然具有挑战性。在此,通过在被(100)面封闭的 Pd 纳米线(NWs)上进行种子合成,制备了具有丰富高能原子台阶(即阶化 Pd)的五孪晶 Pd 纳米线(NWs)。得益于表面上如 [n(100) × m(111)] 的催化活性原子台阶,所得阶化 Pd NWs 可用作直接醇燃料电池(DAFCs)中重要的阳极反应乙醇氧化反应(EOR)和乙二醇氧化反应(EGOR)的有效电催化剂。与商业 Pd/C 相比,由(100)面和原子台阶束缚的 Pd 纳米线对 EOR 和 EGOR 均显示出增强的催化活性和稳定性。重要的是,阶化 Pd NWs 对 EOR 和 EGOR 的质量活性分别为 6.38 和 7.98 A mg,分别是被(100)面封闭的 Pd NWs 的 3.1 和 2.6 倍。此外,我们的合成策略还能够形成具有丰富原子台阶的双金属 Pd-Cu 纳米线。这项工作不仅展示了一种简单而有效的策略,用于获得具有丰富原子台阶的单金属或双金属纳米线,而且还突出了原子台阶在提高电催化剂活性方面的重要作用。

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