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

Abstract

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, hexaazatrinaphthalenequione (HATNQ) is reported for aqueous ZIBs. The HATNQ electrodes delivered an ultrahigh capacity (482.5 mAh g À 1 at 0.2 A g À 1 ) and outstanding cyclability of > 10 000 cycles at 5 A g À 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 π-π 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 Zn 2 + /H + , particularly the storage of Zn 2 + , due to the more favorable O•••Zn•••N coordination in HATNQ.

An Air-Rechargeable Zn/Organic Battery with Proton Storage

“…BQPH was synthesized by Gabriel synthesis and a dehydration condensation reaction (Figure S1). − Its chemical structure and morphology are confirmed by 1 H NMR, 13 C NMR, ESI-MS, FTIR, Raman spectra, SEM, and TEM (Figures S2–S10).…”

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

“…2c). It is worth noting, however, that during preparation of this article, a study 19 reporting the performance of our HATAQ electrode 5 in AZIBs was published, further conrming our results on the excellent electrochemical performance of this material. The highly reversible nature of the redox processes in HATAQ as seen in the electrochemical tests was conrmed by ex situ Fourier-transform infrared (FT-IR) and Raman spectroscopy (Fig.…”

“…The latter reveals the presence of zinc hydroxide sulfate (ZHS) with ake-like morphology on the electrode surface. [18][19][20][21] Scanning transmission electron microscopy (STEM) and energy dispersive X-ray spectroscopy (EDS) analyses were used to perform elemental mapping of HATAQ in the pristine state and at the end of discharge (0.2 V) as shown in Fig. S14.…”

Quantitative analysis of molecular surface: systematic application in the sodiation mechanism of a benzoquinone-based pillared compound as a cathode

“…35 The ESP has been widely used in organic electrode materials for a long time. [36][37][38] However, the ESP values around the ten active sites in P5Q are almost identical due to the high symmetry, which makes it difficult to predict all reaction sites of the whole sodiation process precisely. ALIE and LEA, as essential as the ESP, are closely related to the reactivity and the ability to bind electrons of organic molecules, respectively.…”