Selectively Coupling Ru Single Atoms to PtNi Concavities for High-Performance Methanol Oxidation via d-Band Center Regulation

被引：87
作者：
Kong, Fanpeng [1 ,2 ]
Liu, Xiaozhi [3 ]
Song, Yajie [1 ]
Qian, Zhengyi [1 ]
Li, Junjie [2 ]
Zhang, Lei [2 ]
Yin, Geping [1 ]
Wang, Jiajun [1 ,4 ]
Su, Dong [3 ]
Sun, Xueliang [2 ]
机构：
[1] Harbin Inst Technol, MIIT Key Lab Crit Mat Technol New Energy Convers, Harbin, Peoples R China
[2] Univ Western Ontario, Dept Mech & Mat Engn, London, ON, Canada
[3] Chinese Acad Sci, Inst Phys, Beijing, Peoples R China
[4] Harbin Inst Technol, Chongqing Res Inst, Chongqing, Peoples R China
来源：
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2022年 / 61卷 / 42期
基金：
加拿大创新基金会; 中国国家自然科学基金; 加拿大自然科学与工程研究理事会; 中国博士后科学基金;
关键词：
Concavity; Corrugation; Methanol Oxidation; Operando FTIR; Single Atom; OXYGEN REDUCTION; CARBON-MONOXIDE; PTRU NANOPARTICLES; INITIAL STEPS; CO OXIDATION; PLATINUM; NANOSTRUCTURES; METAL; CATALYST; STRAIN;
D O I：
10.1002/anie.202207524
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
Single atom tailored metal nanoparticles represent a new type of catalysts. Herein, we demonstrate a single atom-cavity coupling strategy to regulate performance of single atom tailored nano-catalysts. Selective atomic layer deposition (ALD) was conducted to deposit Ru single atoms on the surface concavities of PtNi nanoparticles (Ru-ca-PtNi). Ru-ca-PtNi exhibits a record-high activity for methanol oxidation reaction (MOR) with 2.01 A mg(Pt)(-1). Also, Ru-ca-PtNi showcases a significant durability with only 16 % activity loss. Operando electrochemical Fourier transform infrared spectroscopy (FTIR) and theoretical calculations demonstrate Ru single atoms coupled to cavities accelerate the CO removal by regulating d-band center position. Further, the high diffusion barrier of Ru single atoms in concavities accounts for excellent stability. The developed Ru-ca-PtNi via single atom-cavity coupling opens an encouraging pathway to design highly efficient single atom-based (electro)catalysts.
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页数：9
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