Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 142, Issue 46, Pages 19570-19578Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c07992
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Funding
- European Union's Horizon 2020 research and innovation programme [GrapheneCore3 881603]
- ERC Consolidator grant [T2DCP 819698]
- Deutsche Forschungsgemeinschaft (MX-OSMOPED)
- MERA.NET
- Sachsisches Staatsministerium fur Wissenschaft und Kunst [HYSUCAP 100478697]
- German Research Foundation (DFG) within the Cluster of Excellence [CRC 1415, 417590517]
- German Research Foundation (DFG) within the Polymer-based Batteries [SPP 2248]
- Paderborn Center for Parallel Computing (PC2)
- Gauss Centre for Supercomputing e.V.
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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 similar to 66.5 Wh kg(-1)) and supercapacitor-level power densities (133 similar to 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.
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