Tailoring Unsymmetrical-Coordinated Atomic Site in Oxide-Supported Pt Catalysts for Enhanced Surface Activity and Stability

被引:25
|
作者
Xue, Zhenggang [1 ,2 ]
Yan, Muyu [1 ,2 ]
Wang, Xiaolin [3 ]
Wang, Zhiyuan [1 ,2 ]
Zhang, Yan [1 ,2 ]
Li, Yuhuan [4 ,5 ]
Xu, Wenjie [6 ]
Tong, Yujing [1 ,2 ]
Han, Xiao [1 ,2 ]
Xiong, Can [1 ,2 ]
Wang, Wenyu [1 ,2 ]
Chen, Min [1 ,2 ]
Ye, Bangjiao [4 ,5 ]
Hong, Xun [1 ,2 ]
Song, Li [6 ]
Zhang, Hongjun [4 ,5 ]
Yang, Li-Ming [3 ]
Wu, Yuen [1 ,2 ,7 ]
机构
[1] Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Collaborat Innovat Ctr Chem Energy Mat iChEM, Sch Chem & Mat Sci, Hefei 230026, Peoples R China
[2] Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230026, Peoples R China
[3] Huazhong Univ Sci & Technol, Sch Chem & Chem Engn,Hubei Engn Res Ctr Biomat &, Minist Educ,Hubei Key Lab Mat Chem & Serv Failure, Hubei Key Lab Bioinorgan Chem & Mat Med,Key Lab M, Wuhan 430074, Peoples R China
[4] Univ Sci & Technol China, State Key Lab Particle Detect & Elect, Hefei 230026, Peoples R China
[5] Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Peoples R China
[6] Univ Sci & Technol China, Natl Synchrotron Radiat Lab, CAS Ctr Excellence Nanosci, Hefei 230026, Peoples R China
[7] Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
基金
国家重点研发计划; 中国国家自然科学基金;
关键词
nanopockets; nitrogen-assisted defects; oxide-supported Pt catalysts; unsymmetrical coordination; SINGLE; REDUCTION; PLATINUM; TIO2;
D O I
10.1002/smll.202101008
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The catalytic properties of supported metal heterostructures critically depend on the design of metal sites. Although it is well-known that the supports can influence the catalytic activities of metals, precisely regulating the metal-support interactions to achieve highly active and durable catalysts still remain challenging. Here, the authors develop a support effect in the oxide-supported metal monomers (involving Pt, Cu, and Ni) catalysts by means of engineering nitrogen-assisted nanopocket sites. It is found that the nitrogen-permeating process can induce the reconstitution of vacancy interface, resulting in an unsymmetrical atomic arrangement around the vacancy center. The resultant vacancy framework is more beneficial to stabilize Pt monomers and prevent diffusion, which can be further verified by the density functional theory calculations. The final Pt-N/SnO2 catalysts exhibit superior activity and stability for HCHO response (26.5 to 15 ppm). This higher activity allows the reaction to proceed at a lower operating temperature (100 degrees C). Incorporated with wireless intelligent-sensing system, the Pt-N/SnO2 catalysts can further achieve continuous monitoring of HCHO levels and cloud-based terminal data storage.
引用
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页数:7
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