Pt-Embedded CuOx-CeO2 Multicore-Shell Composites: Interfacial Redox Reaction-Directed Synthesis and Composition-Dependent Performance for CO Oxidation

被引:33
|
作者
Wu, Ke [1 ,2 ]
Fu, Xin-Pu [3 ]
Yu, Wen-Zhu [3 ]
Wang, Wei-Wei [3 ]
Jia, Chun-Jiang [3 ]
Du, Pei-Pei [4 ]
Si, Rui [4 ]
Wang, Yu-Hao [1 ,2 ]
Li, Lin-Dong [1 ,2 ]
Zhou, Liang [1 ,2 ]
Sun, Ling-Dong [1 ,2 ]
Yan, Chun-Hua [1 ,2 ,5 ]
机构
[1] Peking Univ, Beijing Natl Lab Mol Sci, State Key Lab Rare Earth Mat Chem & Applicat, PKU HKU Joint Lab Rare Earth Mat & Bioinorgan Che, Beijing 100871, Peoples R China
[2] Peking Univ, Coll Chem & Mol Engn, Beijing 100871, Peoples R China
[3] Shandong Univ, Key Lab Colloid & Interface Chem, Key Lab Special Aggregated Mat, Sch Chem & Chem Engn, Jinan 250100, Shandong, Peoples R China
[4] Chinese Acad Sci, Shanghai Synchrotron Radiat Facil, Shanghai Inst Appl Phys, Shanghai 201204, Peoples R China
[5] Lanzhou Univ, Coll Chem & Chem Engn, Lanzhou 730000, Gansu, Peoples R China
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 embedded CuOx-CeO2 catalyst; interfacial redox reaction; CO oxidation; synergistic catalysis mechanism; metal-support interaction; METAL-SUPPORT INTERACTION; PREFERENTIAL OXIDATION; CATALYTIC PERFORMANCE; CARBON-MONOXIDE; PLATINUM NANOPARTICLES; CEO2; NANOCRYSTALS; CLEAN SYNTHESIS; LATTICE OXYGEN; CRYSTAL PLANE; CERIA;
D O I
10.1021/acsami.8b10496
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
Exploring the state-of-the-art heterogeneous catalysts has been a general concern for sustainable and clean energy. Here, Pt-embedded CuOx-CeO2 multicore-shell (Pt/CuOx-CeO2 MS) composites are fabricated at room temperature via a one-pot and template free procedure for catalyzing CO oxidation, a classical probe reaction, showing a volcano-shaped relationship between the composition and catalytic activity. We experimentally unravel that the Pt/CuOx-CeO2 MS composites are derived from an interfacial autoredox process, where Pt nanoparticles (NPs) are in situ encapsulated by self-assembled ceria nanospheres with CuOx clusters adhered through deposition/precipitation calcination process. Only Cu-O and Pt-Pt coordination structures are determined for CuOx clusters and Pt NPs in Pt/CuOx-CeO2 MS, respectively. Importantly, the close vicinity between Pt and CeO2 benefits to more oxygen vacancies in CeO2 counterparts and results in thin oxide layers on Pt NPs. Meanwhile, the introduction of CuOx clusters is crucial for triggering synergistic catalysis, which leads to high resistance to aggregation of Pt NPs and improvement of catalytic performance. In CO oxidation reaction, both Pt delta+-CO and Cu+-CO can act as active sites during CO adsorption and activation. Nonetheless, redundant content of Pt or Cu will induce a strongly bound Pt-O-Ce or Cu-[O-x]-Ce structures in air-calcinated Pt/CuOx-CeO2 MS composites, respectively, which are both deleterious to catalytic reactivity. As a result, the composition-dependent catalytic activity and superior durability of Pt/CuOx-CeO2 MS composites toward CO oxidation reaction are achieved. This work should be instructive for fabricating desirable multicomponent catalysts composed of noble metal and bimetallic oxide composites for diverse heterogeneous catalysis.
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页码:34172 / 34183
页数:12
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