Isolated Single-Atom Pd Sites in Intermetallic Nanostructures: High Catalytic Selectivity for Semihydrogenation of Alkynes

Feng, Quanchen1; Zhao, Shu1; Wang, Yu2; Dong, Juncai3; Chen, Wenxing1; He, Dongsheng4; Wang, Dingshen1; Yang, Jun5; Zhu, Yuanmin6; Zhu, Hailiang3; Gu, Lin7; Li, Zhi1; Liu, Yuxi5; Yu, Rong6; Li, Jun1; Li, Yadong1

2017-05-31

10.1021/jacs.7b01471

Journal of the American Chemical Society   影响因子和分区

0002-7863

Improving the catalytic selectivity of Pd catalysts is of key importance for various industrial processes and remains a challenge so far. Given the unique properties of single-atom catalysts, isolating contiguous Pd atoms into a single-Pd site with another metal to form intermetallic structures is an effective way to endow Pd with high catalytic selectivity and to stabilize the single site with the intermetallic structures. Based on density functional theory modeling, we demonstrate that the (110) surface of Pm (3) over barm PdIn with single-atom Pd sites shows high selectivity for semihydrogenation of acetylene, whereas the (111) surface of P4/mmm Pd3In with Pd trimer sites shows low selectivity. This idea has been further validated by experimental results that intermetallic PdIn nanocrystals mainly exposing the (110) surface exhibit much higher selectivity for acetylene hydrogenation than Pd3In nanocrystals mainly exposing the (111) surface (92% vs 21% ethylene selectivity at 90 degrees C). This work provides insight for rational design of bimetallic metal catalysts with specific catalytic properties.

SCI ; EI

英语

ESI高被引 ; NI期刊 ; ESI高被引 ; ESI高被引 ; ESI高被引 ; ESI高被引

其他

National Natural Science Foundation of China[21521091]

Chemistry

Chemistry, Multidisciplinary

WOS:000402691800027

AMER CHEMICAL SOC

20172303732367

Acetylene ; Atoms ; Binary alloys ; Catalyst selectivity ; Density functional theory ; Ethylene ; Intermetallics ; Lighting ; Nanocrystals

Metallurgy:531.1 ; Precious Metals:547.1 ; Nanotechnology:761 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Atomic and Molecular Physics:931.3

Web of Science

1.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
2.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrontron Radiat Facil, Shanghai 201204, Peoples R China
3.Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China
4.South Univ Sci & Technol China, Mat Characterizat & Preparat Ctr, Shenzhen 518055, Peoples R China
5.Beijing Univ Technol, Dept Chem & Chem Engn, Beijing 100124, Peoples R China
6.Tsinghua Univ, Beijing Natl Ctr Electron Microscopy, Sch Mat Sci & Engn, Beijing 100084, Peoples R China
7.Chinese Acad Sci, Inst Phys, Beijing 100190, Peoples R China

Feng, Quanchen,Zhao, Shu,Wang, Yu,et al. Isolated Single-Atom Pd Sites in Intermetallic Nanostructures: High Catalytic Selectivity for Semihydrogenation of Alkynes[J]. Journal of the American Chemical Society,2017,139(21):7294-7301.

Feng, Quanchen.,Zhao, Shu.,Wang, Yu.,Dong, Juncai.,Chen, Wenxing.,...&Li, Yadong.(2017).Isolated Single-Atom Pd Sites in Intermetallic Nanostructures: High Catalytic Selectivity for Semihydrogenation of Alkynes.Journal of the American Chemical Society,139(21),7294-7301.

Feng, Quanchen,et al."Isolated Single-Atom Pd Sites in Intermetallic Nanostructures: High Catalytic Selectivity for Semihydrogenation of Alkynes".Journal of the American Chemical Society 139.21(2017):7294-7301.