A dendrite-free and anticaustic Zn anode enabled by high current-induced reconstruction of the electrical double layer

Abstract

Aqueous Zn-based batteries deliver thousands of cycles at high rates but poor recyclability at low rates. Herein, we reveal that such illogical phenomenon is attributed to the reconstructed electrode/electrolyte interface...

Refining the Grain Size of Zinc Electrodeposit by Pb2+ Ion Grinding for Compact and Stable Zinc Anode

“…X‐ray diffraction (XRD) was carried out to find out the deposition orientations. In ZS electrolyte, the Zn electrodeposits showed the relatively strong (101) orientation at the low current density but the relatively strong (002) orientation at the high current density (Figure 2j), which actually experienced a series of current‐induced morphology evolution from irregular plate‐like deposit to plate‐stacked texture with enhanced current density (see details in our previous work [11] ). In this process, the enhanced (002) peak intensity meant that there were more plate‐like (002) planes parallel to the substrate.…”

“…[7,10] Although the dense Zn electrodeposits are able to be formed at the high current densities, the current-dependent regulation strategy is powerless to fundamentally solve the challenges facing Zn anode. [11] Fortunately, the Zn electrodeposits in such a Pb 2 + ion-containing electrolyte were consisted of refined Zn grains at whatever current densities, thereby weaving compact and smooth electrodeposits under all test conditions (Figure 2e-h, and Figure S5e-h, Supporting Information).…”

Reunderstanding aqueous Zn electrochemistry from interfacial specific adsorption of solvation structures

“…27,28,54 Specifically, excess of specific adsorbed anions in IHP will attract more cations in OHP for balancing excess charges from specific adsorbed anions, thus enhancing the kinetics of deposition and denser deposition behavior, namely the ψ 1 effect. 27,28,31,55,56 It is noteworthy that the above analysis shows that the two electrolytes, regardless of the cathode and anode, both exhibit strong specific adsorption of the sulfate-based electrolyte and weak specific adsorption of the sulfonate-based electrolyte, as shown in Scheme 2. For the cathode electrode side, the strong specific adsorption (2S+0.1 electrolyte) might cause irreversible damage to the electrolyte and electrode caused by excessive deposition of MnO 2 , while the weak specific adsorption is conducive to the stability of the cathode (2F+0.1 electrolyte) but shows unsatisfactory capacity performance.…”

High reversibility at high current density: the zinc electrodeposition principle behind the “trick”

“…Lately, Huang et al initiated a discussion regarding the reorganization of a condensed region with tight-absorbed Zn 2+ ions from the perspective of the electrical double layer (EDL). 34 Molecular dynamics (MD) simulations were used to investigate the effect of the high current density operation on the EDL. Surprisingly, the results of this study contradicted the traditional theory of mass-transport limitations, which posits that the ion-deficient layer becomes more pronounced under high-rate conditions.…”