Optimizing the Structure and Electrochemical Properties of Benzoquinone-Embedded COF via Heat Treatment for a High-Energy Organic Cathode
A benzoquinone-embedded aza-fused covalent organic framework (BQ COF) with the maximum loading of redox-active units per molecule was employed as a cathode for lithium-ion batteries (LIBs) to achieve high energy and power densities. The synthesis was optimized to obtain high crystallinity and improved electrochemical performance. Synthesis at moderate temperature followed by a solid-state reaction was found to be particularly useful for achieving good crystallinity and the activation of the COF. When used as a cathode for LIBs, very high discharge capacities of 513, 365, and 234 mAh g-1 were obtained at 0.1C, 1C, and 10C, respectively, showing a remarkable rate performance. More than 70% of the initial capacity was retained after 1000 cycles when the cathode was investigated for cyclic performance at 2.5C. We demonstrated that a straightforward heat treatment led to enhanced crystallinity, an optimized structure, and favorable morphology, resulting in enhanced electrode kinetics and an improved overall electrochemical behavior. A comparative study was conducted involving an aza-fused COF lacking carbonyl groups (TAB COF) and a small molecule containing phenazine and carbonyl (3BQ), providing useful insights into new material design. A full cell was assembled with graphite as the anode to assess the commercial feasibility of BQ COF, and a discharge capacity of 240 mAh g-1 was obtained at 0.5C. Furthermore, a pouch-type cell with a high discharge capacity and an excellent rate performance was assembled, demonstrating the practical applicability of our designed cathode. Considering the entire mass of the working electrode, a specific energy density of 492 Wh kg-1 and a power density of 492 W kg-1 were achieved at the high current density of 1C, which are comparable to those of commercially available cathodes. These results highlight the promise of organic electrode materials for next-generation lithium-ion batteries. Furthermore, this study provides a systematic approach for simultaneously designing organic materials with high power and energy densities.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2023 |
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| Erschienen: |
2023 |
| Enthalten in: |
Zur Gesamtaufnahme - year:2023 |
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| Enthalten in: |
ACS applied materials & interfaces - (2023) vom: 15. Nov. |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Amin, Kamran [VerfasserIn] |
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| Links: |
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| Themen: |
Covalent organic framework |
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| Anmerkungen: |
Date Revised 15.11.2023 published: Print-Electronic Citation Status Publisher |
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| doi: |
10.1021/acsami.3c11998 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| PPN (Katalog-ID): |
NLM364596767 |
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| 024 | 7 | |a 10.1021/acsami.3c11998 |2 doi | |
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| 100 | 1 | |a Amin, Kamran |e verfasserin |4 aut | |
| 245 | 1 | 0 | |a Optimizing the Structure and Electrochemical Properties of Benzoquinone-Embedded COF via Heat Treatment for a High-Energy Organic Cathode |
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| 500 | |a Date Revised 15.11.2023 | ||
| 500 | |a published: Print-Electronic | ||
| 500 | |a Citation Status Publisher | ||
| 520 | |a A benzoquinone-embedded aza-fused covalent organic framework (BQ COF) with the maximum loading of redox-active units per molecule was employed as a cathode for lithium-ion batteries (LIBs) to achieve high energy and power densities. The synthesis was optimized to obtain high crystallinity and improved electrochemical performance. Synthesis at moderate temperature followed by a solid-state reaction was found to be particularly useful for achieving good crystallinity and the activation of the COF. When used as a cathode for LIBs, very high discharge capacities of 513, 365, and 234 mAh g-1 were obtained at 0.1C, 1C, and 10C, respectively, showing a remarkable rate performance. More than 70% of the initial capacity was retained after 1000 cycles when the cathode was investigated for cyclic performance at 2.5C. We demonstrated that a straightforward heat treatment led to enhanced crystallinity, an optimized structure, and favorable morphology, resulting in enhanced electrode kinetics and an improved overall electrochemical behavior. A comparative study was conducted involving an aza-fused COF lacking carbonyl groups (TAB COF) and a small molecule containing phenazine and carbonyl (3BQ), providing useful insights into new material design. A full cell was assembled with graphite as the anode to assess the commercial feasibility of BQ COF, and a discharge capacity of 240 mAh g-1 was obtained at 0.5C. Furthermore, a pouch-type cell with a high discharge capacity and an excellent rate performance was assembled, demonstrating the practical applicability of our designed cathode. Considering the entire mass of the working electrode, a specific energy density of 492 Wh kg-1 and a power density of 492 W kg-1 were achieved at the high current density of 1C, which are comparable to those of commercially available cathodes. These results highlight the promise of organic electrode materials for next-generation lithium-ion batteries. Furthermore, this study provides a systematic approach for simultaneously designing organic materials with high power and energy densities | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a Review | |
| 650 | 4 | |a Covalent organic framework | |
| 650 | 4 | |a Heat treatment | |
| 650 | 4 | |a High energy density battery | |
| 650 | 4 | |a Lithium-ion batteries | |
| 650 | 4 | |a Organic cathode | |
| 700 | 1 | |a Mehmood, Warisha |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Jianqi |e verfasserin |4 aut | |
| 700 | 1 | |a Ahmed, Sadia |e verfasserin |4 aut | |
| 700 | 1 | |a Mao, Lijuan |e verfasserin |4 aut | |
| 700 | 1 | |a Li, Chuan-Fu |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Bin Bin |e verfasserin |4 aut | |
| 700 | 1 | |a Wei, Zhixiang |e verfasserin |4 aut | |
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| 856 | 4 | 0 | |u http://dx.doi.org/10.1021/acsami.3c11998 |3 Volltext |
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