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用于高效乙醇氧化反应的高熵纳米合金的可编程合成

Programmable Synthesis of High-Entropy Nanoalloys for Efficient Ethanol Oxidation Reaction.

作者信息

Li Mengfan, Huang Chenming, Yang Hao, Wang Yu, Song Xiangcong, Cheng Tao, Jiang Jietao, Lu Yangfan, Liu Maochang, Yuan Quan, Ye Zhizhen, Hu Zheng, Huang Hongwen

机构信息

College of Materials Science and Engineering, Hunan University, Changsha, Hunan 410082, People's Republic of China.

Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Jiangsu 215123, People's Republic of China.

出版信息

ACS Nano. 2023 Jul 25;17(14):13659-13671. doi: 10.1021/acsnano.3c02762. Epub 2023 Jul 7.

DOI:10.1021/acsnano.3c02762
PMID:37418375
Abstract

Controllable synthesis of nanoscale high-entropy alloys (HEAs) with specific morphologies and tunable compositions is crucial for exploring advanced catalysts. The present strategies either have great difficulties to tailor the morphology of nanoscale HEAs or suffer from narrow elemental distributions and insufficient generality. To overcome the limitations of these strategies, here we report a robust template-directed synthesis to programmatically fabricate nanoscale HEAs with controllable compositions and structures via independently controlling the morphology and composition of HEA. As a proof of concept, 12 kinds of nanoscale HEAs with controllable morphologies of zero-dimension (0D) nanoparticles, 1D nanowires, 2D ultrathin nanorings (UNRs), 3D nanodendrites, and vast elemental compositions combining five or more of Pd/Pt/Ag/Cu/Fe/Co/Ni/Pb/Bi/Sn/Sb/Ge are synthesized. Moreover, the as-prepared HEA-PdPtCuPbBiUNRs/C demonstrates the state-of-the-art electrocatalytic performance for the ethanol oxidation reaction, with 25.6- and 16.3-fold improvements in mass activity, relative to commercial Pd/C and Pt/C catalysts, respectively, as well as greatly enhanced durability. This work provides a myriad of nanoscale HEAs and a general synthetic strategy, which are expected to have broad impacts for the fields of catalysis, sensing, biomedicine, and even beyond.

摘要

可控合成具有特定形貌和可调组成的纳米级高熵合金(HEA)对于探索先进催化剂至关重要。目前的策略要么在定制纳米级HEA的形貌方面存在很大困难,要么存在元素分布狭窄和通用性不足的问题。为了克服这些策略的局限性,在此我们报告了一种强大的模板导向合成方法,通过独立控制HEA的形貌和组成,以可编程方式制备具有可控组成和结构的纳米级HEA。作为概念验证,合成了12种具有可控形貌的纳米级HEA,包括零维(0D)纳米颗粒、一维纳米线、二维超薄纳米环(UNR)、三维纳米树枝晶,以及包含Pd/Pt/Ag/Cu/Fe/Co/Ni/Pb/Bi/Sn/Sb/Ge中五种或更多种元素组成的大量组合。此外,所制备的HEA-PdPtCuPbBiUNRs/C在乙醇氧化反应中表现出了最先进的电催化性能,相对于商业Pd/C和Pt/C催化剂,质量活性分别提高了25.6倍和16.3倍,并且耐久性也大大增强。这项工作提供了大量的纳米级HEA和一种通用合成策略,预计对催化、传感、生物医学等领域甚至更广泛的领域产生广泛影响。

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