Rechargeable aqueous Zn-ion energy storage devices are promising candidates for next-generation energy storage technologies. However, the lack of highly reversible Zn2+-storage anode materials with low potential windows remains a primary concern. Here, we report a two-dimensional polyarylimide covalent organic framework (PI-COF) anode with high-kinetics Zn2+-storage capability. The well-organized pore channels of PI-COF allow the high accessibility of the build-in redox-active carbonyl groups and efficient ion diffusion with a low energy barrier. The constructed PI-COF anode exhibits a specific capacity (332 C g–1 or 92 mAh g–1 at 0.7 A g–1), a high rate capability (79.8% at 7 A g–1), and a long cycle life (85% over 4000 cycles). In situ Raman investigation and first-principle calculations clarify the two-step Zn2+-storage mechanism, in which imide carbonyl groups reversibly form negatively charged enolates. Dendrite-free full Zn-ion devices are fabricated by coupling PI-COF anodes with MnO2 cathodes, delivering excellent energy densities (23.9 ∼ 66.5 Wh kg–1) and supercapacitor-level power densities (133 ∼ 4782 W kg–1). This study demonstrates the feasibility of covalent organic framework as Zn2+-storage anodes and shows a promising prospect for constructing reliable aqueous energy storage devices.
| Identifer | oai:union.ndltd.org:DRESDEN/oai:qucosa:de:qucosa:79791 |
| Date | 05 July 2022 |
| Creators | Yu, Minghao, Naisa, Chandrasekhar, Raghupathy, Ramya Kormath Madam, Ly, Khoa Hoang, Zhang, Haozhe, Dmitrieva, Evgenia, Liang, Chaolun, Lu, Xihong, Kühne, Thomas D., Mirhosseini, Hossein, Weidinger, Inez M., Feng, Xinliang |
| Publisher | American Chemical Society |
| Source Sets | Hochschulschriftenserver (HSSS) der SLUB Dresden |
| Language | English |
| Detected Language | English |
| Type | info:eu-repo/semantics/acceptedVersion, doc-type:article, info:eu-repo/semantics/article, doc-type:Text |
| Rights | info:eu-repo/semantics/openAccess |
| Relation | 1520-5126, 10.1021/jacs.0c07992, info:eu-repo/grantAgreement/European Commission/H2020 | SGA-RIA/881603//Graphene Flagship Core Project 3/GrapheneCore3, info:eu-repo/grantAgreement/European Commission/H2020 | ERC | ERC-COG/819698//Development of Thiophene Based Conjugated Polymers in Two Dimensions/T2DCP, info:eu-repo/grantAgreement/Deutsche Forschungsgemeinschaft/Sachbeihilfen/399684426//MXen–Organische Halbleiter-Verschnitte mit hohen Ladungsträgermobilitäten für die Anwendung in gedruckter Organischer Elektronik/MX-OSMOPED, info:eu-repo/grantAgreement/Deutsche Forschungsgemeinschaft/Sonderforschungsbereiche/417590517//Chemie der synthetischen zweidimensionalen Materialien/CRC 1415, info:eu-repo/grantAgreement/Deutsche Forschungsgemeinschaft/Schwerpunktprogramm/422726248//Polymer-basierte Batterien/SPP 2248 |
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