Atomic origin of CO-Interaction effect of PtPb@Pt catalyst revealed by in situ environmental transmission electron microscopy

Wang, Qi1,2; Xia, Guang-Jie3,4; Zhao, Zhi Liang1,2; Zhu, Yuanmin1,2,5; Shi, Xiaobo1,2; Huang, Limin3,4; Wang, Yang-Gang3,4; Gu, Meng1,2

2020-10

10.1016/j.nanoen.2020.105099

Nano Energy   影响因子和分区

2211-2855

2211-3282

The carbon monoxide (CO) interaction effect on active Pt-based catalysts is critical because the surface reconstruction and phase separation behavior of bimetallic catalysts in a CO environment can profoundly impact the catalysts' activity and durability. However, because direct and dynamic observation has proven elusive, the exact failure mechanisms of the nanocrystal structural modifications induced by CO are poorly understood. In this work, we probe the dynamic structural and compositional transformations of an individual PtPb@Pt nanoplates in a CO gas atmosphere via in-situ environmental transmission electron microscopy (ETEM) and confirmed with theoretical calculations. The interaction of Pt and Pb atoms with CO molecules are revealed dynamically, including the resulting breakdown of the PtPb@Pt nanoplates. The Pt atoms aggregate on surface facets of the original PtPb lattice and the Pt-CO complex mobilizes, cracking the Pt surface layers and stripping Pb atoms from the PtPb alloy core to form Pb(CO)(4). These interactions provide direct clues for the failure analysis of the catalyst and, thus, represent a critical step towards the design of an anti-CO interaction catalyst.

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The carbon monoxide (CO) interaction effect on active Pt-based catalysts is critical because the surface reconstruction and phase separation behavior of bimetallic catalysts in a CO environment can profoundly impact the catalysts' activity and durability. However, because direct and dynamic observation has proven elusive, the exact failure mechanisms of the nanocrystal structural modifications induced by CO are poorly understood. In this work, we probe the dynamic structural and compositional transformations of an individual PtPb@Pt nanoplates in a CO gas atmosphere via in-situ environmental transmission electron microscopy (ETEM) and confirmed with theoretical calculations. The interaction of Pt and Pb atoms with CO molecules are revealed dynamically, including the resulting breakdown of the PtPb@Pt nanoplates. The Pt atoms aggregate on surface facets of the original PtPb lattice and the Pt-CO complex mobilizes, cracking the Pt surface layers and stripping Pb atoms from the PtPb alloy core to form Pb(CO)(4). These interactions provide direct clues for the failure analysis of the catalyst and, thus, represent a critical step towards the design of an anti-CO interaction catalyst.

;

The carbon monoxide (CO) interaction effect on active Pt-based catalysts is critical because the surface reconstruction and phase separation behavior of bimetallic catalysts in a CO environment can profoundly impact the catalysts' activity and durability. However, because direct and dynamic observation has proven elusive, the exact failure mechanisms of the nanocrystal structural modifications induced by CO are poorly understood. In this work, we probe the dynamic structural and compositional transformations of an individual PtPb@Pt nanoplates in a CO gas atmosphere via in-situ environmental transmission electron microscopy (ETEM) and confirmed with theoretical calculations. The interaction of Pt and Pb atoms with CO molecules are revealed dynamically, including the resulting breakdown of the PtPb@Pt nanoplates. The Pt atoms aggregate on surface facets of the original PtPb lattice and the Pt-CO complex mobilizes, cracking the Pt surface layers and stripping Pb atoms from the PtPb alloy core to form Pb(CO)(4). These interactions provide direct clues for the failure analysis of the catalyst and, thus, represent a critical step towards the design of an anti-CO interaction catalyst.

Co-interaction Surface-composition Ptpb@pt Catalyst Segregation In-situ Tem Pseudopotentials Aimd Reduction Dft Calculation Poison Alloys Shape

SCI ; EI

英语

通讯

National Natural Science Foundation of China[21802065]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied

WOS:000572165000003

ELSEVIER

20202708899942

Platinum alloys ; Platinum compounds ; Carbon monoxide ; Cobalt alloys ; Degradation ; Atoms ; Design for testability ; High resolution transmission electron microscopy ; Catalyst activity ; Failure (mechanical) ; Phase separation ; Nanostructures

Precious Metals:547.1 ; Nonferrous Metals and Alloys excluding Alkali and Alkaline Earth Metals:549.3 ; Thermodynamics:641.1 ; Optical Devices and Systems:741.3 ; Nanotechnology:761 ; Chemical Reactions:802.2 ; Chemical Operations:802.3 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Atomic and Molecular Physics:931.3 ; Solid State Physics:933

Web of Science

1.Dept Mat Sci & Engn, Shenzhen, Guangdong, Peoples R China;
2.Shenzhen Engn Res Ctr Novel Elect Informat Mat &, Shenzhen, Guangdong, Peoples R China;
3.Southern Univ Sci & Technol, Dept Chem, 1088 Xueyuan Blvd, Shenzhen 518055, Guangdong, Peoples R China;
4.Southern Univ Sci & Technol, Guangdong Prov Key Lab Catalysis, 1088 Xueyuan Blvd, Shenzhen 518055, Guangdong, Peoples R China;
5.Southern Univ Sci & Technol, SUSTech Acad Adv Interdisciplinary Studies, Shenzhen 518055, Peoples R China

Wang, Qi,Xia, Guang-Jie,Zhao, Zhi Liang,et al. Atomic origin of CO-Interaction effect of PtPb@Pt catalyst revealed by in situ environmental transmission electron microscopy[J]. Nano Energy,2020,76.

Wang, Qi.,Xia, Guang-Jie.,Zhao, Zhi Liang.,Zhu, Yuanmin.,Shi, Xiaobo.,...&Gu, Meng.(2020).Atomic origin of CO-Interaction effect of PtPb@Pt catalyst revealed by in situ environmental transmission electron microscopy.Nano Energy,76.

Wang, Qi,et al."Atomic origin of CO-Interaction effect of PtPb@Pt catalyst revealed by in situ environmental transmission electron microscopy".Nano Energy 76(2020).