Surface Lattice-Embedded Pt Single-Atom Catalyst on Ceria-Zirconia with Superior Catalytic Performance for Propane Oxidation

被引:28
|
作者
Tan, Wei [1 ,2 ,3 ,4 ]
Xie, Shaohua [1 ]
Cai, Yandi [2 ,3 ,4 ]
Yu, Haowei [2 ,3 ,4 ]
Ye, Kailong [1 ]
Wang, Meiyu [5 ]
Diao, Weijian [6 ]
Ma, Lu [7 ]
Ehrlich, Steven N. [7 ]
Gao, Fei [2 ,3 ,4 ]
Dong, Lin [2 ,3 ,4 ]
Liu, Fudong [1 ]
机构
[1] Univ Cent Florida, NanoSci Technol Ctr NSTC, Dept Civil Environm & Construct Engn, Catalysis Cluster Renewable Energy & Chem Transfor, Orlando, FL 32816 USA
[2] Nanjing Univ, Sch Environm, State Key Lab Pollut Control & Resource Reuse, Nanjing 210023, Peoples R China
[3] Nanjing Univ, Ctr Modern Anal, Jiangsu Key Lab Vehicle Emiss Control, Nanjing 210023, Peoples R China
[4] Nanjing Univ, Sch Chem & Chem Engn, Key Lab Mesoscop Chem MOE, Nanjing 210023, Peoples R China
[5] Nanjing Univ, Coll Engn & Appl Sci, Nanjing 210093, Peoples R China
[6] Villanova Univ, Dept Chem & Biol Engn, Villanova, PA 19085 USA
[7] Brookhaven Natl Lab, Natl Synchrotron Light Source NSLS 2 2, Upton, NY 11973 USA
基金
美国国家科学基金会; 中国国家自然科学基金;
关键词
Pt single atom; calcination temperature; C3H8 oxidation reaction; Pt-CeO2; interaction; coordination environment; CO OXIDATION; ALUMINA CATALYSTS; SCALE VIEW; TEMPERATURE; SUPPORT; OXYGEN; STABILITY; CEO2; IDENTIFICATION; REDUCTION;
D O I
10.1021/acs.est.3c03497
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Ahighly efficient Pt single-atom catalyst was constructedon pre-stabilized Ce0.9Zr0.1O2 supportvia high-temperature calcination for catalytic oxidation of C3H8. Tuning the metal-support interaction and coordinationenvironmentof single-atom catalysts can help achieve satisfactory catalytic performancefor targeted reactions. Herein, via the facile control of calcinationtemperatures for Pt catalysts on pre-stabilized Ce0.9Zr0.1O2 (CZO) support, Pt single atoms (Pt-1) with different strengths of Pt-CeO2 interactionand coordination environment were successfully constructed. With theincrease in calcination temperature from 350 to 750 & DEG;C, a strongerPt-CeO2 interaction and higher Pt-O-Ce coordinationnumber were achieved due to the reaction between PtO x and surface Ce3+ species as well as the migrationof Pt-1 into the surface lattice of CZO. The Pt/CZO catalystcalcined at 750 & DEG;C (Pt/CZO-750) exhibited a surprisingly higherC(3)H(8) oxidation activity than that calcined at550 & DEG;C (Pt/CZO-550). Through systematic characterizations andreaction mechanism study, it was revealed that the higher concentrationof surface Ce3+ species/oxygen vacancies and the strongerPt-CeO2 interaction on Pt/CZO-750 could better facilitatethe activation of oxygen to oxidize C3H8 intoreactive carbonate/carboxyl species and further promote the transformationof these intermediates into gaseous CO2. The Pt/CZO-750catalyst can be a potential candidate for the catalytic removal ofhydrocarbons from vehicle exhaust.
引用
收藏
页码:12501 / 12512
页数:12
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