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作者:

Feng, Quanchen (Feng, Quanchen.) | Zhao, Shu (Zhao, Shu.) | Xu, Qi (Xu, Qi.) | Chen, Wenxing (Chen, Wenxing.) | Tian, Shubo (Tian, Shubo.) | Wang, Yu (Wang, Yu.) | Yan, Wensheng (Yan, Wensheng.) | Luo, Jun (Luo, Jun.) | Wang, Dingsheng (Wang, Dingsheng.) | Li, Yadong (Li, Yadong.)

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摘要:

Semihydrogenation of acetylene in the ethylene feed is a vital step for the industrial production of polyethylene. Despite their favorable reaction activity and ethylene selectivity, the Pd-based intermetallic compound and single-atom alloy catalysts still suffer from the limitation of atomic utilization derived from the partial exposure of active Pd atoms. Herein, a hard-template Lewis acid doping strategy is reported that can overcome the inefficient utilization of Pd atoms. In this strategy, N-coordinated isolated single-atomic Pd sites are fully embedded on the inner walls of mesoporous nitrogen-doped carbon foam nanospheres (ISA-Pd/MPNC). This synthetic strategy has been proved to be applicable to prepare other ISA-M/MPNC (M = Pt and Cu) materials. This ISA-Pd/MPNC catalyst with both high specific surface area (633.8 m(2) g(-1)) and remarkably thin pore wall (1-2 nm) exhibits higher activity than that of its nonmesoporous counterpart (ISA-Pd/non-MPNC) catalyst by a factor of 4. This work presents an efficient way to tailor and optimize the catalytic activity and selectivity by atomic-scale design and structural control.

关键词:

nitrogen-doped carbon semihydrogenation of acetylene palladium mesoporous single-atom catalysts

作者机构:

  • [ 1 ] [Feng, Quanchen]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
  • [ 2 ] [Xu, Qi]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
  • [ 3 ] [Chen, Wenxing]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
  • [ 4 ] [Tian, Shubo]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
  • [ 5 ] [Wang, Dingsheng]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
  • [ 6 ] [Li, Yadong]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
  • [ 7 ] [Zhao, Shu]Beijing Univ Technol, Beijing Guyue New Mat Res Inst, Beijing 100124, Peoples R China
  • [ 8 ] [Wang, Yu]Chinese Acad Sci, Shanghai Synchrotron Radiat Facil, Shanghai Adv Res Inst, Shanghai 201204, Peoples R China
  • [ 9 ] [Yan, Wensheng]Univ Sci & Technol China, Natl Synchrotron Radiat Facil, Hefei 230029, Anhui, Peoples R China
  • [ 10 ] [Luo, Jun]Tianjin Univ Technol, Ctr Electron Microscopy, Tianjin 300384, Peoples R China

通讯作者信息:

  • [Wang, Dingsheng]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China;;[Wang, Yu]Chinese Acad Sci, Shanghai Synchrotron Radiat Facil, Shanghai Adv Res Inst, Shanghai 201204, Peoples R China

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来源 :

ADVANCED MATERIALS

ISSN: 0935-9648

年份: 2019

期: 36

卷: 31

2 9 . 4 0 0

JCR@2022

ESI学科: MATERIALS SCIENCE;

ESI高被引阀值:211

JCR分区:1

被引次数:

WoS核心集被引频次: 175

SCOPUS被引频次: 171

ESI高被引论文在榜: 0 展开所有

万方被引频次:

中文被引频次:

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