Abstract
Rechargeable organic batteries show great potential as a low-cost, sustainable and mass-producible alternatives to current transition-metal-based cells; however, serious electrode dissolution issues and solubilization of organic redox intermediates (shuttle effect) have plagued the capacity retention and cyclability of these cells. Here we report on the use of a metal–organic framework (MOF) gel membrane as a separator for organic batteries. The homogeneous micropores, intrinsic of the MOF-gel separator, act as permselective channels for targeted organic intermediates, thereby mitigating the shuttling problem without sacrificing power. A battery using a MOF-gel separator and 5,5′-dimethyl-2,2′-bis-p-benzoquinone (Me2BBQ) as the electrode displays high cycle stability with capacity retention of 82.9% after 2,000 cycles, corresponding to a capacity decay of ~0.008% per cycle, with a discharge capacity of ~171 mA h g−1 at a current density of 300 mA g−1. The molecular and ionic sieving capabilities of MOF-gel separators promise general applicability, as pore size can be tuned to specific organic electrode materials. The use of MOF-gel separators to prevent side reactions of soluble organic redox intermediates could lead to the development of rechargeable organic batteries with high energy density and long cycling life.
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Acknowledgements
This work was financially supported by the Creative Materials Discovery Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT and Future Planning (NRF-2017M3D1A1039553). This work was also supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIP) (no. 2018R1A2A1A05079249), and project code (IBS-R006-A2). S.B. acknowledges the Korea Research Fellowship (KRF) Program through the National Research Foundation of Korea funded by the Ministry of Science and ICT (project no. 2018H1D3A1A01039450).
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K.K. and S.B. conceived the original idea for this work. S.B. designed and performed the experiments. B.K. performed the DFT calculation and discussed the main idea of the manuscript. C.K. and D.L. helped synthesize the electrode materials of Me2BBQ, BNQ and BHNQ. O.T. helped analyse the SEM images. H.P. helped analyse the ultraviolet–visible spectra. H.P. and J.K. helped the data analysis. S.B. wrote a draft of the manuscript, and K.K. revised it. All of the authors discussed the results of the manuscript. K.K. supervised all of the work.
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Bai, S., Kim, B., Kim, C. et al. Permselective metal–organic framework gel membrane enables long-life cycling of rechargeable organic batteries. Nat. Nanotechnol. 16, 77–84 (2021). https://doi.org/10.1038/s41565-020-00788-x
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DOI: https://doi.org/10.1038/s41565-020-00788-x
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