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.

引用

页数：9

共 53 条

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