4.8 Article

Two-Dimensional Organic Supramolecule via Hydrogen Bonding and π-π Stacking for Ultrahigh Capacity and Long-Life Aqueous Zinc-Organic Batteries

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 37, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202116289

Keywords

Hydrogen Bonding; Organic Cathodes; Organic Zinc-Ion Batteries; pi-pi Stacking; Supramolecules

Funding

  1. National Natural Science Foundation of China [51773071, 52173163]
  2. National 1000-Talents Program
  3. Innovation Fund of WNLO
  4. Fundamental Research Funds for the Central Universities [2019kfyRCPY099]
  5. Open Fund of the State Key Laboratory of Integrated Optoelectronics [IOSKL2020KF02]
  6. Hubei Provincial Natural Science Foundation of China [2019CFA002]
  7. China Postdoctoral Science Foundation [2021TQ0115, 2021M701302, 2020M672323]
  8. HUST Analytical Testing Center

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In this study, a novel cathode material called HATNQ was reported for aqueous zinc-ion batteries (ZIBs). The HATNQ electrodes exhibited ultrahigh capacity and outstanding cycling stability, attributed to its unique 2D layered supramolecular structure and rich functional groups.
Aqueous zinc-ion batteries (ZIBs) are promising for next-generation energy storage. However, the reported electrode materials for ZIBs are facing shortcomings including low capacity and unsatisfactory cycling stability etc. Herein, hexaazatrinaphthalene-quione (HATNQ) is reported for aqueous ZIBs. The HATNQ electrodes delivered an ultrahigh capacity (482.5 mAh g(-1) at 0.2 A g(-1)) and outstanding cyclability of >10 000 cycles at 5 A g(-1). The capacity sets a new record for organic cathodes in aqueous ZIBs. The high performances are ascribed to the rich C=O and C=N groups that endowed HATNQ with a 2D layered supramolecular structure by multiple hydrogen bonds in plane with pi-pi interactions out-of-plane, leading to enhanced charge transfer, insolubility, and rapid ion transport for fast-charge and -discharge batteries. Moreover, the 2D supramolecular structure boosted the storage of Zn2+/H+, particularly the storage of Zn2+, due to the more favorable O center dot center dot center dot Zn center dot center dot center dot N coordination in HATNQ.

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