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Assembly of trimetallic palladium-silver-copper nanosheets for efficient C2 alcohol electrooxidation

用于高效C2醇氧化电催化的三金属钯-银-铜纳米片组装体

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Abstract

The synthesis of two-dimensional (2D) alloyed efficient electrocatalysts with several active sites has attracted considerable attention in recent years. In this work, trimetallic palladium-silver-copper (PdAgCu) nanosheet assemblies (NSAs) are synthesized in the presence of cetyltrimethylammonium bromide and molybdenum hexacarbonyl as the structure-directing agents. The morphologies and structures of the trimetallic PdAgCu NSAs are identified by high-angle annular dark-field scanning transmission electron microscopy, transmission electron microscopy, and X-ray diffraction. The trimetallic Pd6Ag3Cu2 NSA has high electrocatalytic performance with outstanding long-term stabilities for ethylene glycol oxidation reaction (EGOR = 5696 mA mgPd−1) and ethanol oxidation reaction (EOR = 4374 mA mgPd−1). The enhanced electrocatalytic activities can be attributed to the synergistic effects, including strain, ligand, and bifunctional effects. Furthermore, the electrocatalytic mechanisms of the trimetallic electrocatalysts toward C2 alcohols are determined, and high concentrations of OH− and C2 alcohols favor EGOR and EOR.

摘要

近年来, 具有丰富活性中心的二维合金高效电催化剂的合成引 起人们极大关注. 本工作以十六烷基三甲基溴化铵和六羰基钼为结构 导向剂合成出三金属钯-银-铜纳米片组装体. 用高角度环形暗场扫描 透射电子显微镜、透射电子显微镜和X射线衍射仪对三金属PdAgCu纳 米片组装体的形貌和结构进行了表征. 结果表明三金属Pd6Ag3Cu2纳米 片组装体电催化性能优异, 且对乙二醇氧化反应(5696 mA mgPd−1)和乙 醇氧化反应(4374 mA mgPd−1)具有良好的催化稳定性. 电催化活性的增 强可归因于应变效应、配体效应及双功能效应的协同作用. 本文系统 研究了三金属电催化剂对C2醇的电催化机理, 发现较高的羟基和C2醇 浓度有利于乙二醇氧化反应和乙醇氧化反应.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (22172084 and 21773133) and the World-Class Discipline Program of Shandong Province, China.

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  1. These authors contribute equally to this work.

Authors and Affiliations

  1. Institute of Materials for Energy and Environment, College of Materials Science and Engineering, Qingdao University, Qingdao, 266071, China

    Ze Li  (李泽), Xianzhuo Lao  (劳显焯), Likang Yang  (杨立康) & Peizhi Guo  (郭培志)

  2. College of Chemistry and Chemical Engineering, Qingdao University, Qingdao, 266071, China

    Aiping Fu  (傅爱萍)

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  1. Ze Li  (李泽)
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Contributions

Li Z, Lao X, and Guo P conceived and designed the electrocatalysts and experiments. Li Z, Lao X, and Yang L performed the experiments. Li Z, Lao X, Yang L, and Guo P contributed to the analysis of data and the drafting of the article. Lao X and Fu A contributed to the theoretical analysis. All authors discussed and commented on the article.

Corresponding author

Correspondence to Peizhi Guo  (郭培志).

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The authors declare that they have no conflict of interest.

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Supporting data are available in the online version of the paper.

Ze Li is a graduate student in Prof. Peizhi Guo’s group at the School of Materials Science and Engineering, Qingdao University. His current research interests focus on the synthesis and electrocatalytic properties of noble-metalbased nanomaterials.

Xianzhuo Lao is a graduate student in Prof. Peizhi Guo’s group at the School of Materials Science and Engineering, Qingdao University. His current research interests focus on the synthesis and electrocatalytic properties of noblemetal-based nanomaterials.

Peizhi Guo received his BSc degree from Liaocheng University (1998), MSc degree from Shandong University (2003), and PhD degree from the Institute of Chemistry, Chinese Academy of Sciences (2006). He joined Qingdao University as an associate professor in 2006 and became a full professor in 2013. His research interests focus on the design, synthesis, and self-assembly of nanoparticles for electrocatalysis and energy storage.

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Li, Z., Lao, X., Yang, L. et al. Assembly of trimetallic palladium-silver-copper nanosheets for efficient C2 alcohol electrooxidation. Sci. China Mater. 66, 150–159 (2023). https://doi.org/10.1007/s40843-022-2104-4

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