Electrocrystallization Regulation Enabled Stacked Hexagonal Platelet Growth toward Highly Reversible Zinc Anodes

Abstract

Realizing durative flattened and dendrite‐free zinc (Zn) metal configuration is the key to resolving premature battery failure caused by the internal short circuit, which is highly determined by the crystal growth in the electrocrystallization process. Herein, we report that regulating the molecular structure of the inner Helmholtz plane (HIP) can effectively convert the deposition into activation control by weakening the solvated ion adsorption at the interface. The moderated electrochemical reaction kinetics lower than the adatom self‐diffusion rate steers conformal stratiform Zn growth and dominant Zn (0001) texture, achieving crystallographic optimization. Through in situ mediation of electrolyte engineering, orientational plating and stripping behaviors at edge‐sites and tailored solvation structure immensely improve the utilization efficiency and total charge passed of Zn metal, even under extreme conditions, including high areal capacity (3 mAh cm−2) and wide temperature range (−40–60 °C).

Mimicking ion and water management in poultry breeding for highly reversible zinc ion batteries

“…Electrons and Zn 2+ are then inclined to accumulate at the tips of these nonuniform Zn nuclei that eventually evolve into dendrites and dead Zn. 6,8 Moreover, the fast consumption of Zn 2+ on electrode surfaces, especially at high currents, causes Zn 2+ depletion at the interface, increases the overpotential, downgrades the power output, and eventually impairs the overall energy efficiency. 9–11 Overall, a fast and uniform Zn 2+ flow is desirable, which is somewhat controversial to the requirements of water flow management.…”

Advance in Electrolyte for Stable Zinc Anodes in Mild Aqueous Batteries

“…This result is further verified by DFT calculations (Figure d). The designed electrolyte is conductive to significantly increase CE of Zn (>99.7% 1000 cycles, an increase of more than 33 times) . The addition of high-valence cations in ZnSO 4 aqueous solution can weaken the double layer repulsion, facilitate the deposition of dense metal zinc, and regulate the charge distribution at the zinc metal–electrolyte interface.…”

“…(d) Charge density difference diagrams of H 2 O, TMS on the Zn (0001) plane, and their corresponding adsorption energy values. Panels a–d reproduced with permission from ref . Copyright 2023 John Wiley and Sons Ltd.…”

“…The designed electrolyte is conductive to significantly increase CE of Zn (>99.7% 1000 cycles, an increase of more than 33 times). 45 The addition of highvalence cations in ZnSO 4 aqueous solution can weaken the double layer repulsion, facilitate the deposition of dense metal zinc, and regulate the charge distribution at the zinc metal− electrolyte interface. Zhao et al found that electrodeposited Zn in ZS electrolyte tends to grow into independent hexagons due to the EDL repulsive predominant interaction in zinc deposits (Figure 4e).…”

Cellulose-complexing strategy induced surface regulation towards ultrahigh utilization rate of Zn

“…Presently, the strategies employed to prepare stable Zn anodes include electrolyte regulation, surface protection/interface engineering, and Zn anode design. 5,7,8,10,11,13–18 Through the rational design of the electrolyte, Zn 2 coordination can be reconstructed from hexa-hydrated [Zn(H 2 O) 6 ] 2+ , which influences the deposition of Zn, HER and formation of an SEI. Considering that both the free water and solvated water in the electrolyte can trigger water-induced side reactions, 19,20 significant efforts have been devoted to regulating the content of water and its activity in the electrolyte.…”