Electron-Donors-Acceptors Interaction Enhancing Electrocatalytic Activity of Metal-Organic Polymers for Oxygen Reduction
© 2023 Wiley-VCH GmbH..
Catalysts with metal-Nx sites have long been considered as effective electrocatalysts for oxygen reduction reaction (ORR), yet the accurate structure-property correlations of these active sites remain debatable. Report here is a proof-of-concept method to construct 1,4,8,11-tetraaza[14]annulene (TAA)-based polymer nanocomposites with well-managed electronic microenvironment via electron-donors/acceptors interaction of altering electron-withdrawing β-site substituents. DFT calculation proves the optimal -Cl substituted catalyst (CoTAA-ClGR) tailored the key OH* intermediate interaction with Co-N4 sites under the d-orbital regulation, hence reaching the top of ORR performance with excellent turnover frequency (0.49 e s-1 site-1 ). The combination of in situ scanning electrochemical microscopy and variable-frequency square wave voltammetry techniques contribute the great ORR kinetics of CoTAA-Cl@GR to the relatively high accessible site density (7.71×1019 site g-1 ) and fast electron outbound propagation mechanism. This work provides theoretical guidance for rational design of high-performance catalysts for ORR and beyond.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2023 |
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| Erschienen: |
2023 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:62 |
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| Enthalten in: |
Angewandte Chemie (International ed. in English) - 62(2023), 33 vom: 14. Aug., Seite e202306667 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Huang, Bingyu [VerfasserIn] |
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| Links: |
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| Themen: |
Electrocatalyst |
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| Anmerkungen: |
Date Revised 08.08.2023 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1002/anie.202306667 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| PPN (Katalog-ID): |
NLM358802652 |
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| 520 | |a © 2023 Wiley-VCH GmbH. | ||
| 520 | |a Catalysts with metal-Nx sites have long been considered as effective electrocatalysts for oxygen reduction reaction (ORR), yet the accurate structure-property correlations of these active sites remain debatable. Report here is a proof-of-concept method to construct 1,4,8,11-tetraaza[14]annulene (TAA)-based polymer nanocomposites with well-managed electronic microenvironment via electron-donors/acceptors interaction of altering electron-withdrawing β-site substituents. DFT calculation proves the optimal -Cl substituted catalyst (CoTAA-ClGR) tailored the key OH* intermediate interaction with Co-N4 sites under the d-orbital regulation, hence reaching the top of ORR performance with excellent turnover frequency (0.49 e s-1 site-1 ). The combination of in situ scanning electrochemical microscopy and variable-frequency square wave voltammetry techniques contribute the great ORR kinetics of CoTAA-Cl@GR to the relatively high accessible site density (7.71×1019 site g-1 ) and fast electron outbound propagation mechanism. This work provides theoretical guidance for rational design of high-performance catalysts for ORR and beyond | ||
| 650 | 4 | |a Journal Article | |
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| 650 | 4 | |a Electron-Donors-Acceptors | |
| 650 | 4 | |a Oxygen Reduction | |
| 650 | 4 | |a Structure-Property Correlations | |
| 650 | 4 | |a Zinc-Air Battery | |
| 700 | 1 | |a Tang, Xiannong |e verfasserin |4 aut | |
| 700 | 1 | |a Hong, Yaoshuai |e verfasserin |4 aut | |
| 700 | 1 | |a Li, Longbin |e verfasserin |4 aut | |
| 700 | 1 | |a Hu, Ting |e verfasserin |4 aut | |
| 700 | 1 | |a Yuan, Kai |e verfasserin |4 aut | |
| 700 | 1 | |a Chen, Yiwang |e verfasserin |4 aut | |
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