In situ identification of the metallic state of Ag nanoclusters in oxidative dispersion

被引:85
作者
Li, Rongtan [1 ,2 ]
Xu, Xiaoyan [3 ,4 ]
Zhu, Beien [5 ,6 ]
Li, Xiao-Yan [2 ,6 ]
Ning, Yanxiao [1 ]
Mu, Rentao [1 ]
Du, Pengfei [2 ,4 ]
Li, Mengwei [4 ]
Wang, Huike [7 ]
Liang, Jiajie [7 ]
Chen, Yongsheng [8 ]
Gao, Yi [5 ,6 ]
Yang, Bing [3 ,4 ]
Fu, Qiang [1 ,4 ]
Bao, Xinhe [1 ,4 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian, Peoples R China
[2] Univ Chinese Acad Sci, Beijing, Peoples R China
[3] Chinese Acad Sci, Dalian Inst Chem Phys, CAS Key Lab Sci & Technol Appl Catalysis, Dalian, Peoples R China
[4] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian, Peoples R China
[5] Chinese Acad Sci, Interdisciplinary Res Ctr, Shanghai Adv Res Inst, Shanghai, Peoples R China
[6] Chinese Acad Sci, Shanghai Inst Appl Phys, Key Lab Interfacial Phys & Technol, Shanghai, Peoples R China
[7] Nankai Univ, Sch Mat Sci & Engn, Natl Inst Adv Mat, Tianjin, Peoples R China
[8] Nankai Univ, Coll Chem, Key Lab Funct Polymer Mat, Minist Educ, Tianjin, Peoples R China
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
AUGER PARAMETER; ACTIVE-SITES; SILVER; REDISPERSION; CATALYST; CO; NANOPARTICLES; PLATINUM; REGENERATION; CERIA;
D O I
10.1038/s41467-021-21552-2
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Oxidative dispersion has been widely used in regeneration of sintered metal catalysts and fabrication of single atom catalysts, which is attributed to an oxidation-induced dispersion mechanism. However, the interplay of gas-metal-support interaction in the dispersion processes, especially the gas-metal interaction has not been well illustrated. Here, we show dynamic dispersion of silver nanostructures on silicon nitride surface under reducing/oxidizing conditions and during carbon monoxide oxidation reaction. Utilizing environmental scanning (transmission) electron microscopy and near-ambient pressure photoelectron spectroscopy/photoemission electron microscopy, we unravel a new adsorption-induced dispersion mechanism in such a typical oxidative dispersion process. The strong gas-metal interaction achieved by chemisorption of oxygen on nearly-metallic silver nanoclusters is the internal driving force for dispersion. In situ observations show that the dispersed nearly-metallic silver nanoclusters are oxidized upon cooling in oxygen atmosphere, which could mislead to the understanding of oxidation-induced dispersion. We further understand the oxidative dispersion mechanism from the view of dynamic equilibrium taking temperature and gas pressure into account, which should be applied to many other metals such as gold, copper, palladium, etc. and other reaction conditions. Designing ultra small metal nanoclusters or single atoms with metallic state is a challenge. Here, the authors demonstrate the stabilization of ultra small silver clusters in the nearly-metallic state by oxygen adsorption at high temperature, using in situ spectroscopy and microscope technologies.
引用
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页数:9
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