Proton-enabled biomimetic stabilization of small-molecule organic cathode in aqueous zinc-ion batteries

Nhu T.H. Luu, Alexander S. Ivanov, Teng Hao Chen, Ilja Popovs, Jui Chin Lee, Watchareeya Kaveevivitchai

Research output: Contribution to journalArticlepeer-review

18 Scopus citations

Abstract

Small-molecule organic cathode materials offer flexible structural design features, high capacity and sustainable production. Nonetheless, the stability decrease due to the high solubility of the electrode materials especially under electrochemical cycling conditions limits their wide-range applications in energy storage technologies. We describe a nature-inspired strategy to address cathode stability via introduction of transient vinylogous amide hydrogen bond networks into the small-molecule organic electrode material hexaazatrianthranylene (HATA) embedded quinone (HATAQ). Thanks to the proton-enabled biomimetic mechanism, HATAQ exhibits unparalleled cycling stability, ultra-high capacity and rate capability in aqueous zinc-ion batteries, delivering 492 mA h g−1 at 50 mA g−1 and a reversible capacity of 199 mA h g−1, corresponding to 99% retention at 20 A g−1 after 1000 cycles.

Original languageEnglish
Pages (from-to)12371-12377
Number of pages7
JournalJournal of Materials Chemistry A
Volume10
Issue number23
DOIs
StatePublished - May 9 2022

Funding

This work was supported by the Ministry of Science and Technology (MOST) of Taiwan under grant MOST109-2113-M-006-016 (to T.-H. C.) and the Young Scholar Fellowship Program MOST109-2636-E-006-001 (to W. K.). This work was also financially supported by the Hierarchical Green-Energy Materials (Hi-GEM) Research Center, from the Featured Areas Research Center Program within the framework of the Higher Education Sprout Project by the Ministry of Education (MOE) and MOST (MOST109-2634-F-006-020) in Taiwan (to W. K.). This research was supported in part by the High Education Sprout Project, Ministry of Education of the Headquarters of University Advancement at NCKU (to T.-H. C. and W. K.). The computational and scattering work by A. S. I. at Oak Ridge National Laboratory (ORNL) was supported as part of the Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science and Office of Basic Energy Sciences. ORNL is managed by UT-Battelle LLC for the DOE under Contract No. DE-AC05-00OR22725. I. P. was supported by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under contract number DE-AC05-00OR22725. The 28-ID-1 beamline of the National Synchrotron Light Source II was used, which is a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under contract number DE-SC0012704. This research used resources of the Computer and Data Environment for Science (CADES) at ORNL. The authors acknowledge the use of ESCA000200, NMR000700, NMR000800 and EM000800 of MOST110-2731-M-006-001 belonging to the Core Facility Center of NCKU. This manuscript has been authored in part by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (https://energy.gov/downloads/doe-public-access-plan). This work was supported by the Ministry of Science and Technology (MOST) of Taiwan under grant MOST109-2113-M-006-016 (to T.-H. C.) and the Young Scholar Fellowship Program MOST109-2636-E-006-001 (to W. K.). This work was also financially supported by the Hierarchical Green-Energy Materials (Hi-GEM) Research Center, from the Featured Areas Research Center Program within the framework of the Higher Education Sprout Project by the Ministry of Education (MOE) and MOST (MOST109-2634-F-006-020) in Taiwan (to W. K.). This research was supported in part by the High Education Sprout Project, Ministry of Education of the Headquarters of University Advancement at NCKU (to T.-H. C. and W. K.). The computational and scattering work by A. S. I. at Oak Ridge National Laboratory (ORNL) was supported as part of the Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science and Office of Basic Energy Sciences. ORNL is managed by UT-Battelle LLC for the DOE under Contract No. DE-AC05-00OR22725. I. P. was supported by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under contract number DE-AC05-00OR22725. The 28-ID-1 beamline of the National Synchrotron Light Source II was used, which is a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under contract number DE-SC0012704. This research used resources of the Computer and Data Environment for Science (CADES) at ORNL. The authors acknowledge the use of ESCA000200, NMR000700, NMR000800 and EM000800 of MOST110-2731-M-006-001 belonging to the Core Facility Center of NCKU. This manuscript has been authored in part by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( https://energy.gov/downloads/doe-public-access-plan ).

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