Reshaping Dynamics of Gold Nanoparticles under H-2 and O-2 at Atmospheric Pressure
Chmielewski, A; Meng, J; Zhu, BE; Gao, Y; Guesmi, H; Prunier, H; Alloyeau, D; Wang, G; Louis, C; Delannoy, L
刊名ACS NANO
2019
卷号13期号:2页码:2024—2033
关键词LOW-TEMPERATURE OXIDATION SUPPORTED GOLD CATALYTIC-ACTIVITY ELECTRON-MICROSCOPY CO OXIDATION REACTIVE OXYGEN ACTIVE-SITES HYDROGENATION AU ADSORPTION
ISSN号1936-0851
DOI10.1021/acsnano.8b08530
文献子类期刊论文
英文摘要Despite intensive research efforts, the nature of the active sites for O-2 and H-2 adsorption/dissociation by supported gold nanoparticles (NPs) is still an unresolved issue in heterogeneous catalysis. This stems from the absence of a clear picture of the structural evolution of Au NPs at near reaction conditions, i.e., at high pressures and high temperatures. We hereby report real-space observations of the equilibrium shapes of titania-supported Au NPs under O-2 and H-2 at atmospheric pressure using gas transmission electron microscopy. In situ TEM observations show instantaneous changes in the equilibrium shape of Au NPs during cooling under O-2 from 400 degrees C to room temperature. In comparison, no instant change in equilibrium shape is observed under a H-2 environment. To interpret these experimental observations, the equilibrium shape of Au NPs under O-2 atomic oxygen, and H-2 is predicted using a multiscale structure reconstruction model. Excellent agreement between TEM observations and theoretical modeling of Au NPs under O-2 provides strong evidence for the molecular adsorption of oxygen on the Au NPs below 120 degrees C on specific Au facets, which are identified in this work. In the case of H-2, theoretical modeling predicts no interaction with gold atoms that explain their high morphological stability under this gas. This work provides atomic structural information for the fundamental understanding of the O-2 and H-2 adsorption properties of Au NPs under real working conditions and shows a way to identify the active sites of heterogeneous nanocatalysts under reaction conditions by monitoring the structure reconstruction.
语种英语
内容类型期刊论文
源URL[http://ir.sinap.ac.cn/handle/331007/31798]  
专题上海应用物理研究所_中科院上海应用物理研究所2011-2017年
作者单位1.Univ Lyon, Inst Rech Catalyse & Environm Lyon IRCELYON, CNRS, UMR 5256,UCB Lyon 1, 2 Ave Albert Einstein, F-69626 Villeurebanne, France
2.Univ Paris Diderot, Sorbonne Paris Cite, CNRS, Lab Mat & Phenomenes Quant,UMR 7162, F-75013 Paris, France;
3.Chinese Acad Sci, Shanghai Inst Appl Phys, Div Interfacial Water, Shanghai 201800, Peoples R China;
4.Chinese Acad Sci, Shanghai Inst Appl Phys, Key Lab Interfacial Phys & Technol, Shanghai 201800, Peoples R China;
5.Univ Chinese Acad Sci, Beijing 100049, Peoples R China;
6.UM, CNRS, ENSCM, Inst Charles Gerhardt Montpellier, 240 Ave Prof Emile Jeanbrau, F-34090 Montpellier, France;
7.Sorbonne Univ, CNRS, LRS, F-75252 Paris, France;
推荐引用方式
GB/T 7714
Chmielewski, A,Meng, J,Zhu, BE,et al. Reshaping Dynamics of Gold Nanoparticles under H-2 and O-2 at Atmospheric Pressure[J]. ACS NANO,2019,13(2):2024—2033.
APA Chmielewski, A.,Meng, J.,Zhu, BE.,Gao, Y.,Guesmi, H.,...&Nelayah, J.(2019).Reshaping Dynamics of Gold Nanoparticles under H-2 and O-2 at Atmospheric Pressure.ACS NANO,13(2),2024—2033.
MLA Chmielewski, A,et al."Reshaping Dynamics of Gold Nanoparticles under H-2 and O-2 at Atmospheric Pressure".ACS NANO 13.2(2019):2024—2033.
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