Self‐Smoothing Deposition Behavior Enabled by Beneficial Potential Compensating for Highly Reversible Zn‐Metal Anodes

Abstract

Realizing compact dendrite‐free zinc (Zn) plating is crucial to avoiding premature battery failure caused by internal short‐circuits, which is highly determined by the interface electric field (ψi) distribution. Herein, a concept of “potential compensating” is shown on Zn anodes to stimulate its self‐smoothing deposition behavior for durable batteries. A homogeneous ψi with elevated potential intensity is successfully built at the Zn/electrolyte interface via the selective adsorption of highly polarized propylene glycol (PG) molecules, which facilitate the formation of dense and uniform Zn electroplating patterns. Moreover, the PG additive can simultaneously reshape the structure of Zn2+‐solvation sheath and immobilize the H‐bonding networks in bulk electrolyte, enabling Zn anodes with exceptional electrochemical reversibility (99.6%) and ultralong calendar life (3500 h), as revealed by joint spectroscopic and electrochemical analyses. More importantly, full cells with PG safeguard can deliver desirable cycling stability even at an elevated temperature (50 °C) and low N/P ratios (cathode mass loading up to 14.38 mg cm−2). This study presents new insight into the rational design of stable practical electrolytes and interfacial chemistry regulation for sustainable zinc batteries.

Bio-inspired hydroxyl-rich electrolyte additive for highly reversible aqueous Zn-ion batteries with strong coordination chemistry

“…With the import of l -Aa, the cycling life of Zn//Zn symmetric cells at high current density achieves a larger improvement compared with previous results with different additives. 13,14,28,34,54,57–64 The findings presented herein provide compelling evidence that the incorporation of l -Aa can yield a substantial development in the electrochemical reversibility of Zn anodes.…”

“…The variation (band a) of the SO 4 2− stretching mode ( v (SO 4 2− )) at ∼1100 cm −1 authentically verifies the reconstructed Zn 2+ solvation structure in the l -Aa-modified electrolyte. 54 Importantly, although significant numbers of SO 4 2− are associated with Zn 2+ that causes the presence of ZnSO 4 at the interface both with/without l -Aa electrolytes, the vibration intensity of v (SO 4 2− ) in the l -Aa-modified electrolyte is attenuated, which could be attributed to the rearranged coordination structure, possibly facilitating the formation ZnS with l -Aa. To demonstrate the efficacy of the l -Aa additive in mitigating side reactions and controlling morphology evolution, the zinc plating behavior was investigated using both in situ optical microscopy and ex situ X-ray photoelectron spectroscopy (XPS), thereby visualizing the enhancement effect.…”

A Self‐Regulated Interface Enabled by Multi‐Functional pH Buffer for Reversible Zn Electrochemistry

“…[55,56] Then the current density increases and stabilizes due to electrostatic shielding effect of APS additive, which restrains the plane diffusion of Zn 2+ in the 2D range. [29,57] This may be attributed to the fact that surfaceabsorbed NH 4…”

Hierarchical Porous N-Doped Carbon Nanofibers with Encapsulated Li3VO4 Nanoparticles for Lithium-Ion Storage

“…In recent research, significant efforts have been devoted to exploring alternative anodes for LIBs. These materials include Si, Bi, Sn, and their chemical compounds as alloying-type anodes, as well as CoS 2 , MnO, and FeSe 2 as conversion-type anodes. − Additionally, modifications have been made to graphite and Li 4 Ti 5 O 12 anodes to enhance their intercalation properties. − It is well known that anode materials with alloying and conversion reactions generally exhibit higher specific theoretical capacities. However, the large volume variation during Li + insertion/extraction processes can lead to structural degradation and poor cycling stability. , On the other hand, intercalation-type anode materials typically have lower capacities but offer stable structures with minimal volume change.…”