{"title":"Electroactive Tetrathiafulvalene-Based Covalent Organic Framework with Thiophene Units as Anode for High-Performance Hybrid Lithium-Ion Capacitors","authors":"Zhi-Mei Yang, Yaoda Wang, Meng-Hang Zhang, Zhe-Yuan Hou, Shu-Peng Zhao, Xiao Han, Shuai Yuan, Jian Su, Zhong Jin, Jing-Lin Zuo","doi":"10.1016/j.ensm.2025.104038","DOIUrl":null,"url":null,"abstract":"Enhancing the performance of hybrid lithium-ion capacitors (HLICs) by regulating the structural characteristics of covalent organic frameworks (COFs) has been a challenge. In this study, electron-rich thiophene units combining with the electroactive tetrathiafulvalene (TTF) motif consists the designable organic linker, tetrathiafulvalene tetrathiophenal (TTFTTA). A novel 2D COF, TTFTTA-PDA (PDA, <em>p</em>-phenylenediamine), was assembled via a solvothermal method. TTFTTA-PDA exhibits reversible redox activity, a large Brunauer−Emmett−Teller surface area (457 m<sup>2</sup> g<sup>−1</sup>) and high stability (pH 3∼14). Furthermore, compared to the reported tetrathiafulvalene-tetrabenzaldehyde (TTFTBA)-based COF, TTFTBA-PDA, the introduction of thiophene rings enhances the capability of electron transfer, characterized by a smaller band gap (1.45 eV) and a lower calculated energy gap (0.89 eV). As a result, the electrochemical performance of TTFTTA-PDA in HLICs is outstanding. In the full-cell configurations, TTFTTA-PDA||activated carbon HLICs exhibit impressive energy density (140 Wh kg<sup>−1</sup> at 233 W kg<sup>−1</sup>), power density (9328 W kg<sup>−1</sup> at 91 Wh kg<sup>−1</sup>), and cycling lifespan (the capacity retention of 81.3% after 2200 cycles), demonstrating a certain level of competitiveness among the reported state-of-the-art HLICs utilizing metal organic framework-/COF-based anode materials. These results illustrate that the precise structural design of pristine COFs can be an effective strategy to enhancing the performance of HLICs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"45 1","pages":""},"PeriodicalIF":18.9000,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Energy Storage Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1016/j.ensm.2025.104038","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Enhancing the performance of hybrid lithium-ion capacitors (HLICs) by regulating the structural characteristics of covalent organic frameworks (COFs) has been a challenge. In this study, electron-rich thiophene units combining with the electroactive tetrathiafulvalene (TTF) motif consists the designable organic linker, tetrathiafulvalene tetrathiophenal (TTFTTA). A novel 2D COF, TTFTTA-PDA (PDA, p-phenylenediamine), was assembled via a solvothermal method. TTFTTA-PDA exhibits reversible redox activity, a large Brunauer−Emmett−Teller surface area (457 m2 g−1) and high stability (pH 3∼14). Furthermore, compared to the reported tetrathiafulvalene-tetrabenzaldehyde (TTFTBA)-based COF, TTFTBA-PDA, the introduction of thiophene rings enhances the capability of electron transfer, characterized by a smaller band gap (1.45 eV) and a lower calculated energy gap (0.89 eV). As a result, the electrochemical performance of TTFTTA-PDA in HLICs is outstanding. In the full-cell configurations, TTFTTA-PDA||activated carbon HLICs exhibit impressive energy density (140 Wh kg−1 at 233 W kg−1), power density (9328 W kg−1 at 91 Wh kg−1), and cycling lifespan (the capacity retention of 81.3% after 2200 cycles), demonstrating a certain level of competitiveness among the reported state-of-the-art HLICs utilizing metal organic framework-/COF-based anode materials. These results illustrate that the precise structural design of pristine COFs can be an effective strategy to enhancing the performance of HLICs.
期刊介绍:
Energy Storage Materials is a global interdisciplinary journal dedicated to sharing scientific and technological advancements in materials and devices for advanced energy storage and related energy conversion, such as in metal-O2 batteries. The journal features comprehensive research articles, including full papers and short communications, as well as authoritative feature articles and reviews by leading experts in the field.
Energy Storage Materials covers a wide range of topics, including the synthesis, fabrication, structure, properties, performance, and technological applications of energy storage materials. Additionally, the journal explores strategies, policies, and developments in the field of energy storage materials and devices for sustainable energy.
Published papers are selected based on their scientific and technological significance, their ability to provide valuable new knowledge, and their relevance to the international research community.