A High-Rate Two-Dimensional Polyarylimide Covalent Organic Framework Anode for Aqueous Zn-Ion Energy Storage Devices Yu, Minghao Chandrasekhar, Naisa Kormath Madam Raghupathy, Ramya Ly, Khoa Hoang Zhang, Haozhe Dmitrieva, Evgenia Liang, Chaolun Lu, Xihong Kühne, Thomas Mirhosseini, S. Hossein Weidinger, Inez M. Feng, Xinliang 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. American Chemical Society 2020 info:eu-repo/semantics/article doc-type:article text http://purl.org/coar/resource_type/c_6501 https://ris.uni-paderborn.de/record/21240 Yu M, Chandrasekhar N, Kormath Madam Raghupathy R, et al. A High-Rate Two-Dimensional Polyarylimide Covalent Organic Framework Anode for Aqueous Zn-Ion Energy Storage Devices. <i>Journal of the American Chemical Society</i>. 2020;142(46):19570-19578. doi:<a href="https://doi.org/10.1021/jacs.0c07992">10.1021/jacs.0c07992</a> eng info:eu-repo/semantics/altIdentifier/doi/10.1021/jacs.0c07992 info:eu-repo/semantics/altIdentifier/issn/0002-7863 info:eu-repo/semantics/closedAccess