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作者:

Wei, Shengjie (Wei, Shengjie.) | Li, Ang (Li, Ang.) (学者:李昂) | Liu, Jin-Cheng (Liu, Jin-Cheng.) | Li, Zhi (Li, Zhi.) | Chen, Wenxing (Chen, Wenxing.) | Gong, Yue (Gong, Yue.) | Zhang, Qinghua (Zhang, Qinghua.) | Cheong, Weng-Chon (Cheong, Weng-Chon.) | Wang, Yu (Wang, Yu.) | Zheng, Lirong (Zheng, Lirong.) | Xiao, Hai (Xiao, Hai.) | Chen, Chen (Chen, Chen.) | Wang, Dingsheng (Wang, Dingsheng.) | Peng, Qing (Peng, Qing.) | Gu, Lin (Gu, Lin.) | Han, Xiaodong (Han, Xiaodong.) (学者:韩晓东) | Li, Jun (Li, Jun.) | Li, Yadong (Li, Yadong.)

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摘要:

Single noble metal atoms and ultrafine metal clusters catalysts tend to sinter into aggregated particles at elevated temperatures, driven by the decrease of metal surface free energy. Herein, we report an unexpected phenomenon that noble metal nanoparticles (Pd, Pt, Au-NPs) can be transformed to thermally stable single atoms (Pd, Pt, Au-SAs) above 900 degrees C in an inert atmosphere. The atomic dispersion of metal single atoms was confirmed by aberration-corrected scanning transmission electron microscopy and X-ray absorption fine structures. The dynamic process was recorded by in situ environmental transmission electron microscopy, which showed competing sintering and atomization processes during NP-to-SA conversion. Further, density functional theory calculations revealed that high-temperature NP-to-SA conversion was driven by the formation of the more thermodynamically stable Pd-N-4 structure when mobile Pd atoms were captured on the defects of nitrogen-doped carbon. The thermally stable single atoms (Pd-SAs) exhibited even better activity and selectivity than nanoparticles (Pd-NPs) for semi-hydrogenation of acetylene.

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作者机构:

  • [ 1 ] [Wei, Shengjie]Tsinghua Univ, Dept Chem, Beijing, Peoples R China
  • [ 2 ] [Liu, Jin-Cheng]Tsinghua Univ, Dept Chem, Beijing, Peoples R China
  • [ 3 ] [Li, Zhi]Tsinghua Univ, Dept Chem, Beijing, Peoples R China
  • [ 4 ] [Chen, Wenxing]Tsinghua Univ, Dept Chem, Beijing, Peoples R China
  • [ 5 ] [Cheong, Weng-Chon]Tsinghua Univ, Dept Chem, Beijing, Peoples R China
  • [ 6 ] [Xiao, Hai]Tsinghua Univ, Dept Chem, Beijing, Peoples R China
  • [ 7 ] [Chen, Chen]Tsinghua Univ, Dept Chem, Beijing, Peoples R China
  • [ 8 ] [Wang, Dingsheng]Tsinghua Univ, Dept Chem, Beijing, Peoples R China
  • [ 9 ] [Peng, Qing]Tsinghua Univ, Dept Chem, Beijing, Peoples R China
  • [ 10 ] [Li, Jun]Tsinghua Univ, Dept Chem, Beijing, Peoples R China
  • [ 11 ] [Li, Yadong]Tsinghua Univ, Dept Chem, Beijing, Peoples R China
  • [ 12 ] [Li, Ang]Beijing Univ Technol, Beijing Key Lab Microstruct & Property Adv Mat, Beijing, Peoples R China
  • [ 13 ] [Han, Xiaodong]Beijing Univ Technol, Beijing Key Lab Microstruct & Property Adv Mat, Beijing, Peoples R China
  • [ 14 ] [Gong, Yue]Chinese Acad Sci, Beijing Natl Lab Condensed Matter Phys, Inst Phys, Beijing, Peoples R China
  • [ 15 ] [Zhang, Qinghua]Chinese Acad Sci, Beijing Natl Lab Condensed Matter Phys, Inst Phys, Beijing, Peoples R China
  • [ 16 ] [Gu, Lin]Chinese Acad Sci, Beijing Natl Lab Condensed Matter Phys, Inst Phys, Beijing, Peoples R China
  • [ 17 ] [Wang, Yu]Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai, Peoples R China
  • [ 18 ] [Zheng, Lirong]Chinese Acad Sci, Beijing Synchrotron Radiat Facil, Inst High Energy Phys, Beijing, Peoples R China

通讯作者信息:

  • [Li, Zhi]Tsinghua Univ, Dept Chem, Beijing, Peoples R China;;[Li, Yadong]Tsinghua Univ, Dept Chem, Beijing, Peoples R China

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来源 :

NATURE NANOTECHNOLOGY

ISSN: 1748-3387

年份: 2018

期: 9

卷: 13

页码: 856-,

3 8 . 3 0 0

JCR@2022

ESI学科: MATERIALS SCIENCE;

ESI高被引阀值:260

JCR分区:1

被引次数:

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