材料科学
纳米点
纳米结构
兴奋剂
纳米技术
退火(玻璃)
电化学
石墨烯
贵金属
纳米材料
化学工程
金属
光电子学
电极
冶金
化学
工程类
物理化学
作者
Liuxuan Luo,Cehuang Fu,Yangge Guo,Xiyang Cai,Xiashuang Luo,Zehao Tan,Rui Xue,Xiaojing Cheng,Shuiyun Shen,Junliang Zhang
出处
期刊:ACS Nano
[American Chemical Society]
日期:2023-01-27
卷期号:17 (3): 2992-3006
被引量:30
标识
DOI:10.1021/acsnano.2c11627
摘要
Rationally combining designed supports and metal-based nanomaterials is effective to synergize their respective physicochemical and electrochemical properties for developing highly active and stable/durable electrocatalysts. Accordingly, in this work, sub-5 nm and monodispersed nanodots (NDs) with the special nanostructure of an ultrafine Cu1Au1 core and a 2-3-atomic-layer Cu1Pd3 shell are synthesized by a facile solvothermal method, which are further evenly and firmly anchored onto 3D porous N-doped graphene nanosheets (NGS) via a simple annealing (A) process. The as-obtained Cu1Au1@Cu1Pd3 NDs/NGS-A exhibits exceptional electrocatalytic activity and noble-metal utilization toward the alkaline oxygen reduction, methanol oxidation, and ethanol oxidation reactions, showing dozens-fold enhancements compared with commercial Pd/C and Pt/C. Besides, it also has excellent long-term electrochemical stability and electrocatalytic durability. Advanced and comprehensive experimental and theoretical analyses unveil the synthetic mechanism of the special core@shell nanostructure and further reveal the origins of the significantly enhanced electrocatalytic performance: (1) the prominent structural properties of NGS, (2) the ultrasmall and monodispersed size as well as the highly uniform morphology of the NDs-A, (3) the special Cu-Au-Pd alloy nanostructure with an ultrafine core and a subnanometer shell, and (4) the strong metal-support interaction. This work not only develops a facile method for fabricating the special metal-based ultrafine-core@ultrathin-shell nanostructure but also proposes an effective and practical design paradigm of comprehensively and rationally considering both supports and metal-based nanomaterials for realizing high-performance multifunctional electrocatalysts, which can be further expanded to other supports and metal-based nanomaterials for other energy-conversion or environmental (electro)catalytic applications.
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