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作者:

Sun, Tingting (Sun, Tingting.) | Zhao, Shu (Zhao, Shu.) | Chen, Wenxing (Chen, Wenxing.) | Zhai, Dong (Zhai, Dong.) | Dong, Juncai (Dong, Juncai.) | Wang, Yu (Wang, Yu.) | Zhang, Shaolong (Zhang, Shaolong.) | Han, Aijuan (Han, Aijuan.) | Gu, Lin (Gu, Lin.) | Yu, Rong (Yu, Rong.) | Wen, Xiaodong (Wen, Xiaodong.) | Ren, Hanlin (Ren, Hanlin.) | Xu, Lianbin (Xu, Lianbin.) | Chen, Chen (Chen, Chen.) | Peng, Qing (Peng, Qing.) | Wang, Dingsheng (Wang, Dingsheng.) | Li, Yadong (Li, Yadong.)

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摘要:

Exploring efficient and cost-effective catalysts to replace precious metal catalysts, such as Pt, for electrocatalytic oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) holds great promise for renewable energy technologies. Herein, we prepare a type of Co catalyst with single-atomic Co sites embedded in hierarchically ordered porous N-doped carbon (Co-SAS/HOPNC) through a facile dual-template cooperative pyrolysis approach. The desirable combination of highly dispersed isolated atomic Co-N-4 active sites, large surface area, high porosity, and good conductivity gives rise to an excellent catalytic performance. The catalyst exhibits outstanding performance for ORR in alkaline medium with a half-wave potential (E-1/2) of 0.892 V, which is 53 mV more positive than that of Pt/C, as well as a high tolerance of methanol and great stability. The catalyst also shows a remarkable catalytic performance for HER with distinctly high turnover frequencies of 0.41 and 3.8 s(-1) at an overpotential of 100 and 200 mV, respectively, together with a long-term durability in acidic condition. Experiments and density functional theory (DFT) calculations reveal that the atomically isolated single Co sites and the structural advantages of the unique 3D hierarchical porous architecture synergistically contribute to the high catalytic activity.

关键词:

single-atomic cobalt sites oxygen reduction reaction hydrogen evolution reaction in situ XAS measurements hierarchically ordered porous structure

作者机构:

  • [ 1 ] [Sun, Tingting]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
  • [ 2 ] [Chen, Wenxing]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
  • [ 3 ] [Zhang, Shaolong]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
  • [ 4 ] [Han, Aijuan]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
  • [ 5 ] [Ren, Hanlin]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
  • [ 6 ] [Chen, Chen]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
  • [ 7 ] [Peng, Qing]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
  • [ 8 ] [Wang, Dingsheng]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
  • [ 9 ] [Li, Yadong]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
  • [ 10 ] [Zhao, Shu]Beijing Univ Technol, Beijing Guyue New Mat Res Inst, Beijing 100124, Peoples R China
  • [ 11 ] [Zhai, Dong]Shanghai Univ, Mat Genome Inst, Shanghai 200444, Peoples R China
  • [ 12 ] [Zhai, Dong]Shanghai Univ, Int Ctr Quantum & Mol Struct, Dept Phys, Shanghai 200444, Peoples R China
  • [ 13 ] [Dong, Juncai]Chinese Acad Sci, Beijing Synchrotron Radiat Facil, Inst High Energy Phys, Beijing 100049, Peoples R China
  • [ 14 ] [Wang, Yu]Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrontron Radiat Facil, Shanghai 201800, Peoples R China
  • [ 15 ] [Gu, Lin]Chinese Acad Sci, Beijing Natl Lab Condensed Matter Phys, Inst Phys, Beijing 100190, Peoples R China
  • [ 16 ] [Yu, Rong]Tsinghua Univ, Beijing Natl Ctr Electron Microscopy, Sch Mat Sci & Engn, Beijing 100084, Peoples R China
  • [ 17 ] [Wen, Xiaodong]Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Shanxi, Peoples R China
  • [ 18 ] [Xu, Lianbin]Beijing Univ Chem Technol, State Key Lab Organ Inorgan Composites, Beijing 100029, Peoples R China

通讯作者信息:

  • [Wang, Dingsheng]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China;;[Li, Yadong]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China;;[Wang, Yu]Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrontron Radiat Facil, Shanghai 201800, Peoples R China

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来源 :

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA

ISSN: 0027-8424

年份: 2018

期: 50

卷: 115

页码: 12692-12697

1 1 . 1 0 0

JCR@2022

ESI学科: Multidisciplinary;

ESI高被引阀值:337

JCR分区:1

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WoS核心集被引频次: 347

SCOPUS被引频次: 334

ESI高被引论文在榜: 29 展开所有

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