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作者:

Wang, Cong (Wang, Cong.) | Wang, Kaiwen (Wang, Kaiwen.) | Feng, Yibo (Feng, Yibo.) | Li, Chong (Li, Chong.) | Zhou, Xiaoyuan (Zhou, Xiaoyuan.) | Gan, Liyong (Gan, Liyong.) | Feng, Yajie (Feng, Yajie.) | Zhou, Hanjun (Zhou, Hanjun.) | Zhang, Bin (Zhang, Bin.) | Qu, Xianlin (Qu, Xianlin.) | Li, Hui (Li, Hui.) | Li, Jieyuan (Li, Jieyuan.) | Li, Ang (Li, Ang.) (学者:李昂) | Sun, Yiyang (Sun, Yiyang.) | Zhang, Shengbai (Zhang, Shengbai.) | Yang, Guo (Yang, Guo.) | Guo, Yizhong (Guo, Yizhong.) | Yang, Shize (Yang, Shize.) | Zhou, Tianhua (Zhou, Tianhua.) | Dong, Fan (Dong, Fan.) | Zheng, Kun (Zheng, Kun.) | Wang, Lihua (Wang, Lihua.) | Huang, Jun (Huang, Jun.) | Zhang, Ze (Zhang, Ze.) | Han, Xiaodong (Han, Xiaodong.)

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摘要:

The platinum single-atom-catalyst is verified as a very successful route to approach the size limit of Pt catalysts, while how to further improve the catalytic efficiency of Pt is a fundamental scientific question and is challenging because the size issue of Pt is approached at the ultimate ceiling as single atoms. Here, a new route for further improving Pt catalytic efficiency by cobalt (Co) and Pt dual-single-atoms on titanium dioxide (TiO2) surfaces, which contains a fraction of nonbonding oxygen-coordinated Co-O-Pt dimers, is reported. These Co-Pt dimer sites originate from loading high-density Pt single-atoms and Co single-atoms, with them anchoring randomly on the TiO2 substrate. This dual-single-atom catalyst yields 13.4% dimer sites and exhibits an ultrahigh and stable photocatalytic activity with a rate of 43.467 mmol g(-1) h(-1) and external quantum efficiency of approximate to 83.4% at 365 nm. This activity far exceeds those of equal amounts of Pt single-atom and typical Pt clustered catalysts by 1.92 and 1.64 times, respectively. The enhancement mechanism relies on the oxygen-coordinated Co-O-Pt dimer coupling, which can mutually optimize the electronic states of both Pt and Co sites to weaken H* binding. Namely, the "mute" Co single-atom is activated by Pt single-atom and the activity of the Pt atom is further enhanced through the dimer interaction. This strategy of nonbonding interactive dimer sites and the oxygen-mediated catalytic mechanisms provide emerging rich opportunities for greatly improving the catalytic efficiency and developing novel catalysts with creating new electronic states.

关键词:

(2) photocatalysts single&#8208 dual single&#8208 TiO coordination atoms atomic&#8208 site catalysts hydrogen evolution reaction oxygen&#8208

作者机构:

  • [ 1 ] [Wang, Cong]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Adv Mat, Beijing 100124, Peoples R China
  • [ 2 ] [Wang, Kaiwen]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Adv Mat, Beijing 100124, Peoples R China
  • [ 3 ] [Feng, Yibo]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Adv Mat, Beijing 100124, Peoples R China
  • [ 4 ] [Qu, Xianlin]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Adv Mat, Beijing 100124, Peoples R China
  • [ 5 ] [Li, Hui]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Adv Mat, Beijing 100124, Peoples R China
  • [ 6 ] [Li, Ang]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Adv Mat, Beijing 100124, Peoples R China
  • [ 7 ] [Yang, Guo]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Adv Mat, Beijing 100124, Peoples R China
  • [ 8 ] [Guo, Yizhong]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Adv Mat, Beijing 100124, Peoples R China
  • [ 9 ] [Zheng, Kun]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Adv Mat, Beijing 100124, Peoples R China
  • [ 10 ] [Wang, Lihua]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Adv Mat, Beijing 100124, Peoples R China
  • [ 11 ] [Huang, Jun]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Adv Mat, Beijing 100124, Peoples R China
  • [ 12 ] [Zhang, Ze]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Adv Mat, Beijing 100124, Peoples R China
  • [ 13 ] [Han, Xiaodong]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Adv Mat, Beijing 100124, Peoples R China
  • [ 14 ] [Li, Chong]Zhengzhou Univ, Int Lab Quantum Funct Mat Henan, Zhengzhou 450001, Peoples R China
  • [ 15 ] [Li, Chong]Zhengzhou Univ, Sch Phys & Microelect, Zhengzhou 450001, Peoples R China
  • [ 16 ] [Zhou, Xiaoyuan]Chongqing Univ, Coll Phys, Chongqing 400044, Peoples R China
  • [ 17 ] [Gan, Liyong]Chongqing Univ, Coll Phys, Chongqing 400044, Peoples R China
  • [ 18 ] [Feng, Yajie]Chongqing Univ, Coll Phys, Chongqing 400044, Peoples R China
  • [ 19 ] [Zhou, Hanjun]Chongqing Univ, Coll Phys, Chongqing 400044, Peoples R China
  • [ 20 ] [Zhang, Bin]Chongqing Univ, Coll Phys, Chongqing 400044, Peoples R China
  • [ 21 ] [Zhou, Xiaoyuan]Chongqing Univ, Analyt & Testing Ctr, Chongqing 401331, Peoples R China
  • [ 22 ] [Gan, Liyong]Chongqing Univ, Analyt & Testing Ctr, Chongqing 401331, Peoples R China
  • [ 23 ] [Feng, Yajie]Chongqing Univ, Analyt & Testing Ctr, Chongqing 401331, Peoples R China
  • [ 24 ] [Zhou, Hanjun]Chongqing Univ, Analyt & Testing Ctr, Chongqing 401331, Peoples R China
  • [ 25 ] [Zhang, Bin]Chongqing Univ, Analyt & Testing Ctr, Chongqing 401331, Peoples R China
  • [ 26 ] [Li, Jieyuan]Univ Elect Sci & Technol China, Inst Fundamental & Frontier Sci, Chengdu 611731, Peoples R China
  • [ 27 ] [Dong, Fan]Univ Elect Sci & Technol China, Inst Fundamental & Frontier Sci, Chengdu 611731, Peoples R China
  • [ 28 ] [Sun, Yiyang]Chinese Acad Sci, Shanghai Inst Ceram, State Key Lab High Performance Ceram & Superfine, Shanghai 201899, Peoples R China
  • [ 29 ] [Zhang, Shengbai]Rensselaer Polytech Inst, Dept Phys Appl Phys & Astron, Troy, NY 12180 USA

通讯作者信息:

  • 李昂

    [Li, Ang]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Adv Mat, Beijing 100124, Peoples R China;;[Zhou, Xiaoyuan]Chongqing Univ, Coll Phys, Chongqing 400044, Peoples R China;;[Zhou, Xiaoyuan]Chongqing Univ, Analyt & Testing Ctr, Chongqing 401331, Peoples R China

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来源 :

ADVANCED MATERIALS

ISSN: 0935-9648

年份: 2021

期: 13

卷: 33

2 9 . 4 0 0

JCR@2022

ESI学科: MATERIALS SCIENCE;

ESI高被引阀值:116

JCR分区:1

被引次数:

WoS核心集被引频次: 184

SCOPUS被引频次:

ESI高被引论文在榜: 16 展开所有

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