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作者:

Qin, Yi (Qin, Yi.) | Chuang, Cheng-Hao (Chuang, Cheng-Hao.) | Liu, Xiaojing (Liu, Xiaojing.) | Liang, Xian (Liang, Xian.) | Xie, Linfeng (Xie, Linfeng.) | Wang, Kuan (Wang, Kuan.) | Pao, Chih-Wen (Pao, Chih-Wen.) | Lu, Ying-Rui (Lu, Ying-Rui.) | Liu, Yang (Liu, Yang.) | Chen, Yawei (Chen, Yawei.) | Lei, Zhanwu (Lei, Zhanwu.) | Yan, Pengfei (Yan, Pengfei.) | Wu, Liang (Wu, Liang.) | Jiao, Shuhong (Jiao, Shuhong.) | Li, Qing (Li, Qing.) | Cao, Ruiguo (Cao, Ruiguo.)

收录:

EI Scopus SCIE

摘要:

Molecular catalysts have attracted significant attention because of their high activity, selectivity, and tunability. However, in heterogeneous catalysis, the uniform dispersion and immobilization of molecular catalysts on the supporting substrate remain a significant challenge due to their aggregation tendency. Here, we present a facile strategy to molecularly disperse and immobilize a series of macrocyclic metal complexes onto reduced graphene oxide (rGO) by using DNA as a mediator. The electroactive amounts of molecularly dispersed iron phthalocyanine (FePc) molecules are increased by similar to 50 times greater than that of pristine FePc catalyst. As a result, the single-molecule catalyst demonstrates a notable power density (similar to 290 mW cm(-2)) in an H-2/O-2 alkaline polymer electrolyte fuel cell. Operando X-ray absorption spectroscopy experiments combined with density functional theory calculations reveal that the coordination interaction between FePc and DNA enables the molecular dispersion and immobilization of FePc on the surface of rGO, and consequently improves the activity by regulating the electronic structure of active centers. This study points out a facile strategy to tackle the fundamental challenges facing molecular catalysts in long-lasting energy conversion technologies.

关键词:

iron phthalocyanine DNA energy conversion single-molecule catalysts H-2/O-2 alkaline fuel cell

作者机构:

  • [ 1 ] [Qin, Yi]Univ Sci & Technol China, Sch Chem & Mat Sci, Hefei Natl Lab Phys Sci Microscale, CAS Key Lab Mat Energy Convers, Hefei 230026, Peoples R China
  • [ 2 ] [Liu, Yang]Univ Sci & Technol China, Sch Chem & Mat Sci, Hefei Natl Lab Phys Sci Microscale, CAS Key Lab Mat Energy Convers, Hefei 230026, Peoples R China
  • [ 3 ] [Chen, Yawei]Univ Sci & Technol China, Sch Chem & Mat Sci, Hefei Natl Lab Phys Sci Microscale, CAS Key Lab Mat Energy Convers, Hefei 230026, Peoples R China
  • [ 4 ] [Lei, Zhanwu]Univ Sci & Technol China, Sch Chem & Mat Sci, Hefei Natl Lab Phys Sci Microscale, CAS Key Lab Mat Energy Convers, Hefei 230026, Peoples R China
  • [ 5 ] [Jiao, Shuhong]Univ Sci & Technol China, Sch Chem & Mat Sci, Hefei Natl Lab Phys Sci Microscale, CAS Key Lab Mat Energy Convers, Hefei 230026, Peoples R China
  • [ 6 ] [Cao, Ruiguo]Univ Sci & Technol China, Sch Chem & Mat Sci, Hefei Natl Lab Phys Sci Microscale, CAS Key Lab Mat Energy Convers, Hefei 230026, Peoples R China
  • [ 7 ] [Chuang, Cheng-Hao]Tamkang Univ, Dept Phys, New Taipei City 25137, Taiwan
  • [ 8 ] [Chuang, Cheng-Hao]Tamkang Univ, Res Ctr Xray Sci, New Taipei City 25137, Taiwan
  • [ 9 ] [Liu, Xiaojing]Shandong Univ, Inst Frontier & Interdisciplinary Sci, Qingdao 266237, Peoples R China
  • [ 10 ] [Liang, Xian]Univ Sci & Technol China, Collaborat Innovat Ctr Chem Energy Mat, Sch Chem & Mat Sci, CAS Key Lab Soft Matter Chem, Hefei 230026, Peoples R China
  • [ 11 ] [Wu, Liang]Univ Sci & Technol China, Collaborat Innovat Ctr Chem Energy Mat, Sch Chem & Mat Sci, CAS Key Lab Soft Matter Chem, Hefei 230026, Peoples R China
  • [ 12 ] [Xie, Linfeng]Huazhong Univ Sci & Technol, Sch Mat Sci & Engn, State Key Lab Mat Proc & Die & Mould Technol, Wuhan 430074, Peoples R China
  • [ 13 ] [Li, Qing]Huazhong Univ Sci & Technol, Sch Mat Sci & Engn, State Key Lab Mat Proc & Die & Mould Technol, Wuhan 430074, Peoples R China
  • [ 14 ] [Wang, Kuan]Beijing Univ Technol, Fac Mat & Mfg, Beijing Key Lab Microstruct & Properties Solids, Beijing 100124, Peoples R China
  • [ 15 ] [Yan, Pengfei]Beijing Univ Technol, Fac Mat & Mfg, Beijing Key Lab Microstruct & Properties Solids, Beijing 100124, Peoples R China
  • [ 16 ] [Pao, Chih-Wen]Natl Synchrotron Radiat Res Ctr, Hsinchu 300, Taiwan
  • [ 17 ] [Lu, Ying-Rui]Natl Synchrotron Radiat Res Ctr, Hsinchu 300, Taiwan

通讯作者信息:

  • [Lei, Zhanwu]Univ Sci & Technol China, Sch Chem & Mat Sci, Hefei Natl Lab Phys Sci Microscale, CAS Key Lab Mat Energy Convers, Hefei 230026, Peoples R China;;[Cao, Ruiguo]Univ Sci & Technol China, Sch Chem & Mat Sci, Hefei Natl Lab Phys Sci Microscale, CAS Key Lab Mat Energy Convers, Hefei 230026, Peoples R China;;[Li, Qing]Huazhong Univ Sci & Technol, Sch Mat Sci & Engn, State Key Lab Mat Proc & Die & Mould Technol, Wuhan 430074, Peoples R China;;

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来源 :

ACS CATALYSIS

ISSN: 2155-5435

年份: 2024

期: 10

卷: 14

页码: 7514-7525

1 2 . 9 0 0

JCR@2022

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SCOPUS被引频次: 6

ESI高被引论文在榜: 0 展开所有

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