Tuning Carbon Defect in Copper Single-Atom Catalysts for Efficient Oxygen Reduction
© 2023 Wiley-VCH GmbH..
Defect chemistry in carbon matrix shows great potential for promoting the oxygen reduction reaction (ORR) of metal single-atom catalysts. Herein, a modified pyrolysis strategy is proposed to tune carbon defects in copper single-atom catalysts (Cu-SACs) to fully understand their positive effect on the ORR activity. The optimized Cu-SACs with controllable carbon defect degree and enhanced active specific surface area can exhibit improved ORR activity with a half-wave potential of 0.897 VRHE , ultrahigh limiting current density of 6.5 mA cm-2 , and superior turnover frequency of 2.23 e site-1 s-1 . The assembled Zn-air batteries based on Cu-SACs can also show well-retained reversibility and voltage platform over 1100 h charge/discharge period. Density functional theory calculations reveal that suitable carbon defects can redistribute charge density of Cu-N4 active sites to weaken the O-O bond in adsorbed OOH* intermediate and thus reduce its dissociation energy. This discovery offers a universal strategy for fabricating superior single-atom catalysts with high-efficiency active sites toward energy-directed applications.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2023 |
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| Erschienen: |
2023 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:19 |
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| Enthalten in: |
Small (Weinheim an der Bergstrasse, Germany) - 19(2023), 28 vom: 06. Juli, Seite e2301075 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Yao, Xiuyun [VerfasserIn] |
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| Links: |
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| Themen: |
Carbon defects |
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| Anmerkungen: |
Date Completed 12.07.2023 Date Revised 18.07.2023 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1002/smll.202301075 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| PPN (Katalog-ID): |
NLM354832018 |
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| 500 | |a Citation Status PubMed-not-MEDLINE | ||
| 520 | |a © 2023 Wiley-VCH GmbH. | ||
| 520 | |a Defect chemistry in carbon matrix shows great potential for promoting the oxygen reduction reaction (ORR) of metal single-atom catalysts. Herein, a modified pyrolysis strategy is proposed to tune carbon defects in copper single-atom catalysts (Cu-SACs) to fully understand their positive effect on the ORR activity. The optimized Cu-SACs with controllable carbon defect degree and enhanced active specific surface area can exhibit improved ORR activity with a half-wave potential of 0.897 VRHE , ultrahigh limiting current density of 6.5 mA cm-2 , and superior turnover frequency of 2.23 e site-1 s-1 . The assembled Zn-air batteries based on Cu-SACs can also show well-retained reversibility and voltage platform over 1100 h charge/discharge period. Density functional theory calculations reveal that suitable carbon defects can redistribute charge density of Cu-N4 active sites to weaken the O-O bond in adsorbed OOH* intermediate and thus reduce its dissociation energy. This discovery offers a universal strategy for fabricating superior single-atom catalysts with high-efficiency active sites toward energy-directed applications | ||
| 650 | 4 | |a Journal Article | |
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| 650 | 4 | |a carbon defects | |
| 650 | 4 | |a charge density | |
| 650 | 4 | |a oxygen reduction reaction | |
| 650 | 4 | |a single-atom catalysts | |
| 700 | 1 | |a Zhu, Youqi |e verfasserin |4 aut | |
| 700 | 1 | |a Xia, Tianyu |e verfasserin |4 aut | |
| 700 | 1 | |a Han, Zhanli |e verfasserin |4 aut | |
| 700 | 1 | |a Du, Changliang |e verfasserin |4 aut | |
| 700 | 1 | |a Yang, Lifen |e verfasserin |4 aut | |
| 700 | 1 | |a Tian, Jiachen |e verfasserin |4 aut | |
| 700 | 1 | |a Ma, Xilan |e verfasserin |4 aut | |
| 700 | 1 | |a Hou, Jianhua |e verfasserin |4 aut | |
| 700 | 1 | |a Cao, Chuanbao |e verfasserin |4 aut | |
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