Reversible loss of core-shell structure for Ni-Au bimetallic nanoparticles during CO2 hydrogenation

Zhang, Xiaoben1,2; Han, Shaobo3; Zhu, Beien4,5,6; Zhang, Guanghui7,8; Li, Xiaoyan2,5,6; Gao, Yi4,5,6; Wu, Zhaoxuan1; Yang, Bing1; Liu, Yuefeng1; Baaziz, Walid9; Ersen, Ovidiu9; Gu, Meng3; Miller, Jeffrey T.8; Liu, Wei1

2020-03-23

10.1038/s41929-020-0440-2

Nature Catalysis   影响因子和分区

2520-1158

The high catalytic performance of core-shell nanoparticles is usually attributed to their distinct geometric and electronic structures. Here we reveal a dynamic mechanism that overturns this conventional understanding by a direct environmental transmission electron microscopy visualization coupled with multiple state-of-the-art in situ techniques, which include synchrotron X-ray absorption spectroscopy, infrared spectroscopy and theoretical simulations. A Ni-Au catalytic system, which exhibits a highly selective CO production in CO2 hydrogenation, features an intact ultrathin Au shell over the Ni core before and after the reaction. However, the catalytic performance could not be attributed to the Au shell surface, but rather to the formation of a transient reconstructed alloy surface, promoted by CO adsorption during the reaction. The discovery of such a reversible transformation urges us to reconsider the reaction mechanism beyond the stationary model, and may have important implications not only for core-shell nanoparticles, but also for other well-defined nanocatalysts.

SCI ; EI

英语

ESI高被引

通讯

NSFC[21802065]

Chemistry

Chemistry, Physical

WOS:000521527900003

NATURE PUBLISHING GROUP

20201708503777

Gold ; Electronic structure ; Infrared spectroscopy ; Carbon dioxide ; X ray absorption spectroscopy ; Nanocatalysts ; Shells (structures) ; High resolution transmission electron microscopy ; Nanoparticles

Structural Members and Shapes:408.2 ; Precious Metals:547.1 ; Optical Devices and Systems:741.3 ; Nanotechnology:761 ; Chemical Reactions:802.2 ; Inorganic Compounds:804.2 ; Atomic and Molecular Physics:931.3 ; Solid State Physics:933

Web of Science

1.Chinese Acad Sci, DICP, Dalian Natl Lab Clean Energy, Dalian, Peoples R China
2.Univ Chinese Acad Sci, Beijing, Peoples R China
3.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen, Peoples R China
4.Chinese Acad Sci, Shanghai Adv Res Inst, Zhangjiang Lab, Shanghai, Peoples R China
5.Chinese Acad Sci, Shanghai Inst Appl Phys, Div Interfacial Water, Shanghai, Peoples R China
6.Chinese Acad Sci, Shanghai Inst Appl Phys, Key Lab Interfacial Phys & Technol, Shanghai, Peoples R China
7.Dalian Univ Technol, Sch Chem Engn, PSU DUT Joint Ctr Energy Res, State Key Lab Fine Chem, Dalian, Liaoning, Peoples R China
8.Purdue Univ, Davidson Sch Chem Engn, W Lafayette, IN 47907 USA
9.Univ Strasbourg, CNRS, IPCMS, UMR 7504, Strasbourg, France

Zhang, Xiaoben,Han, Shaobo,Zhu, Beien,et al. Reversible loss of core-shell structure for Ni-Au bimetallic nanoparticles during CO2 hydrogenation[J]. Nature Catalysis,2020,3(4):411-417.

Zhang, Xiaoben.,Han, Shaobo.,Zhu, Beien.,Zhang, Guanghui.,Li, Xiaoyan.,...&Liu, Wei.(2020).Reversible loss of core-shell structure for Ni-Au bimetallic nanoparticles during CO2 hydrogenation.Nature Catalysis,3(4),411-417.

Zhang, Xiaoben,et al."Reversible loss of core-shell structure for Ni-Au bimetallic nanoparticles during CO2 hydrogenation".Nature Catalysis 3.4(2020):411-417.