Hydrogen Bond‐Functionalized Massive Solvation Modules Stabilizing Bilateral Interfaces

Abstract

Although mild aqueous electrolytes endow zinc‐ion batteries with intrinsic security surpassing that of lithium‐ion batteries, whether irreversible zinc deposition and related corrosion on the anode or cathode species dissolution severely circumscribes their cyclic stability, especially at low current density. Here, hydrogen bond‐functionalized massive solvation modules in a maltose‐based hybrid electrolyte are constructed, which is crucial for the stability of bilateral interfaces in the cycling process, to address this infamous issue. The intensive solvated interactions and diffusion hindrance effect yield uniform deposition of zinc at the anode interface, while the hydrogen bond confinement to free water interdicts derived parasitic reactions. As for the cathode interface, the massive solvation modules avoid structural framework collapse from vanadium dissolution and preserve low interfacial activation energy during cycling. The above bilateral interface regulation enables resultant full batteries to unprecedentedly maintain 84.2% of its initial specific capacity after 400 continuous cycles even at a very low current density of 50 mA g–1. This work provides a new perspective toward economical and eco‐friendly electrolytes for stable aqueous batteries.

Balanced Interfacial Ion Concentration and Migration Steric Hindrance Promoting High‐Efficiency Deposition/Dissolution Battery Chemistry

“…The v (OH) band located at 2800–3750 cm −1 is deconvoluted into four modules, where the OH 1 and OH 2 units refer to the coupling vibrations between water molecules and the stretching vibrations between hydroxyl group and the nearest molecules, the OH 3 and OH 4 signify the OH stretching vibrations of water molecules with broken hydrogen bonds (Figure 4c). [ 38 ] The basically unchanged peaks indicate that carboxylic anions do not interact with water molecules. In addition, by adding carboxylic acid to MnSO 4 solution, the UV–vis spectrum results, as shown in Figure S13, Supporting Information, exhibit that the addition of formic acid will significantly reduce the intensity of peaks, and the chemical environment of MnSO 4 in acetic acid and propionic acid is more similar to that in pure solution.…”

Interface Reversible Electric Field Regulated by Amphoteric Charged Protein-Based Coating Toward High-Rate and Robust Zn Anode

“…The initial N, O, and S elements of Zn-SF electrodes before cycles (Fig. S13a-c) can be attributed to the SF coating [ 59 ]. After cycles, a weak Zn (II) signal and unchanged S/O elements were detected on the cycled Zn-SF surface, indicating few formations of ZHS.…”

Recent advances and perspectives for Zn-based batteries: Zn anode and electrolyte

“…It participates in reconstructing the solvated shell of Zn 2+ ions, forming a larger coordination structure size. This hydrogen-bonding functional H2O molecule limitation mechanism substantially regulates their electrochemical behavior at the interface [135]. The hydrogen bond-functionalized massive solvation module guides interfacial stability during cycling, which greatly ensures the cycle life of the full cell.…”