Supramolecular Self-Assembled Multi-Electron-Acceptor Organic Molecule as High-Performance Cathode Material for Li-Ion Batteries

Meng Siou Wu, Nhu T.H. Luu, Teng Hao Chen, Hailong Lyu, Te Wei Huang, Sheng Dai, Xiao Guang Sun, Alexander S. Ivanov, Jui Chin Lee, Ilja Popovs, Watchareeya Kaveevivitchai

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69 Scopus citations

Abstract

Organic electrode materials possess many advantages such as low toxicity, sustainability, and chemical/structural tunability toward high energy density. However, to compete with inorganic-based compounds, crucial aspects such as redox potential, capacity, cycling stability, and electronic conductivity need to be improved. Herein, a comprehensive strategy on the molecular design of small organic electron-acceptor-molecule—hexaazatrianthranylene (HATA) embedded quinone (HATAQ) is reported. By introducing conjugated quinone moieties into the electron-deficient hexaazatriphenylene-derivative core, HATAQ with highly extended π-conjugation can yield extra-high capacity for lithium storage, delivering a capacity of 426 mAh g−1 at 200 mA g−1 (0.4C). At an extremely high rate of 10 A g−1 (19C), a reversible capacity of 209 mAh g−1 corresponding to nearly 85% retention is obtained after 1000 cycles. A unique network of unconventional lock-and-key hydrogen bonds in the solid-state facilitates favorable supramolecular 2D layered arrangement, enhancing cycling stability. To the best of the authors’ knowledge, the capacity and rate capability of HATAQ are found to be the best ever reported for organic small-molecule-based cathodes. These results together with density functional theory studies provide proof-of-concept that the design strategy is promising for the development of organic electrodes with exceptionally high energy density, rate capability, and cycling stability.

Original languageEnglish
Article number2100330
JournalAdvanced Energy Materials
Volume11
Issue number31
DOIs
StatePublished - Aug 19 2021

Funding

This work was supported by the Ministry of Science and Technology of Taiwan under grant MOST108-2113-M-006-016 (to T.-H.C.) and the Young Scholar Fellowship Program MOST108-2636-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 the Ministry of Science and Technology (MOST 109-2634-F-006-020) in Taiwan (to W.K.). This research was supported in part by High Education Sprout Project, Ministry of Education of the Headquarters of University Advancement at National Cheng Kung University (NCKU) (to T.-H.C. and W.K.). The research of H.L., X.-G.S., S.D., A.S.I., and I.P. was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under contract number DE-AC05-00OR22725. This research used resources of the Computer and Data Environment for Science (CADES) at Oak Ridge National Laboratory, managed by UT-Battelle, LLC for the U.S. DOE under Contract DE-AC05-00OR22725. The authors gratefully acknowledge the use of ESCA000200 and NMR000700 of MOST 108-2731-M-006-001 belonging to the Core Facility Center of NCKU. The authors are indebted to Dr. Ting-Shen Kuo (National Taiwan Normal University) for the collection and the refinement of crystallographic data, and are grateful to Tsung-Lun Kan (Instrument Center, NCKU) for assisting with NMR data collection. Authors thank the University of Texas at Austin Mass Spectrometry Facility staff for acquiring high resolution mass spectra. This work was supported by the Ministry of Science and Technology of Taiwan under grant MOST108‐2113‐M‐006‐016 (to T.‐H.C.) and the Young Scholar Fellowship Program MOST108‐2636‐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 the Ministry of Science and Technology (MOST 109‐2634‐F‐006‐020) in Taiwan (to W.K.). This research was supported in part by High Education Sprout Project, Ministry of Education of the Headquarters of University Advancement at National Cheng Kung University (NCKU) (to T.‐H.C. and W.K.). The research of H.L., X.‐G.S., S.D., A.S.I., and I.P. was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under contract number DE‐AC05‐00OR22725. This research used resources of the Computer and Data Environment for Science (CADES) at Oak Ridge National Laboratory, managed by UT‐Battelle, LLC for the U.S. DOE under Contract DE‐AC05‐00OR22725. The authors gratefully acknowledge the use of ESCA000200 and NMR000700 of MOST 108‐2731‐M‐006‐001 belonging to the Core Facility Center of NCKU. The authors are indebted to Dr. Ting‐Shen Kuo (National Taiwan Normal University) for the collection and the refinement of crystallographic data, and are grateful to Tsung‐Lun Kan (Instrument Center, NCKU) for assisting with NMR data collection. Authors thank the University of Texas at Austin Mass Spectrometry Facility staff for acquiring high resolution mass spectra.

Keywords

  • Li-ion batteries
  • organic cathode materials
  • supramolecular assemblies

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