Modulating the Electronic Metal-Support Interactions in Single-Atom Pt1-CuO Catalyst for Boosting Acetone Oxidation

被引:71
作者
Jiang, Zeyu [1 ,2 ]
Tian, Mingjiao [1 ,3 ]
Jing, Meizan [4 ]
Chai, Shouning [1 ]
Jian, Yanfei [1 ]
Chen, Changwei [1 ]
Douthwait, Mark [5 ]
Zhen, Lirong [6 ]
Ma, Mudi [1 ]
Song, Weiyu [4 ]
Liu, Jian [4 ]
Yu, Jiaguo [3 ]
He, Chi [1 ,7 ]
机构
[1] Xi An Jiao Tong Univ, State Key Lab Multiphase Flow Power Engn, Xian 710049, Shaanxi, Peoples R China
[2] Natl Univ Singapore, Dept Chem, Singapore 117543, Singapore
[3] China Univ Geosci, Fac Mat Sci & Chem, Lab Solar Fuel, Wuhan 430074, Peoples R China
[4] China Univ Petr, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China
[5] Cardiff Univ, Max Planck Cardiff Ctr Fundamentals Heterogeneous, Sch Chem, Cardiff CF10 3AT, Wales
[6] Chinese Acad Sci, Inst High Energy Phys, Beijing 100049, Peoples R China
[7] Univ Chinese Acad Sci, Natl Engn Lab VOCs Pollut Control Mat & Technol, Beijing 101408, Peoples R China
基金
中国国家自然科学基金;
关键词
Acetone Oxidation; Electronic Metal-Support Interactions; Intrinsic Mechanism; Single-Atom Catalysts; METHYL-ETHYL-KETONE; CO OXIDATION; NANOPARTICLES; FORMALDEHYDE; METHANOL; TRANSFORMATION; ACTIVATION; REDUCTION; SITE;
D O I
10.1002/anie.202200763
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The development of highly active single-atom catalysts (SACs) and identifying their intrinsic active sites in oxidizing industrial hazardous hydrocarbons are challenging prospects. Tuning the electronic metal-support interactions (EMSIs) is valid for modulating the catalytic performance of SACs. We propose that the modulation of the EMSIs in a Pt-1-CuO SAC significantly promotes the activity of the catalyst in acetone oxidation. The EMSIs promote charge redistribution through the unified Pt-O-Cu moieties, which modulates the d-band structure of atomic Pt sites, and strengthens the adsorption and activation of reactants. The positively charged Pt atoms are superior for activating acetone at low temperatures, and the stretched Cu-O bonds facilitate the activation of lattice oxygen atoms to participate in subsequent oxidation. We believe that this work will guide researchers to engineer efficient SACs for application in hydrocarbon oxidation reactions.
引用
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页数:9
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