A π-interactive additive unlocks enhanced zinc anode rechargeability: unveiling the critical role of adsorption layer dynamics

Shang, Y; Ding, Y; Kokate, R; Rana, A; Dick, JE; Wu, X; Hoex, B; Wang, M; Wang, N; Zhang, Q; Kumar, P; Kundu, D

A π-interactive additive unlocks enhanced zinc anode rechargeability: unveiling the critical role of adsorption layer dynamics

Shang, Y Ding, Y Kokate, R Rana, A Dick, JE Wu, X Hoex, B Wang, M Wang, N Zhang, Q Kumar, P Kundu, D

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Publisher:: Royal Society of Chemistry (RSC)
Publication Type:: Journal Article
Citation:: Energy and Environmental Science, 2025, 18, (24), pp. 10523-10536
Issue Date:: 2025-12-21

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Field	Value	Language
dc.contributor.author	Shang, Y
dc.contributor.author	Ding, Y
dc.contributor.author	Kokate, R
dc.contributor.author	Rana, A
dc.contributor.author	Dick, JE
dc.contributor.author	Wu, X
dc.contributor.author	Hoex, B
dc.contributor.author	Wang, M
dc.contributor.author	Wang, N
dc.contributor.author	Zhang, Q
dc.contributor.author	Kumar, P
dc.contributor.author	Kundu, D
dc.date.accessioned	2026-05-19T05:15:56Z
dc.date.available	2026-05-19T05:15:56Z
dc.date.issued	2025-12-21
dc.identifier.citation	Energy and Environmental Science, 2025, 18, (24), pp. 10523-10536
dc.identifier.issn	1754-5692
dc.identifier.issn	1754-5706
dc.identifier.uri	http://hdl.handle.net/10453/195063
dc.description.abstract	Aqueous zinc-ion batteries are promising for a safe, inexpensive, and sustainable platform for stationary energy storage, but their reversibility remains limited by dendrite and corrosion-mediated failure of the zinc anode. While low-concentration electrolyte additives have emerged as scalable solutions, the mechanistic underpinnings of their interfacial dynamics that dictate whether they enable long-term rechargeability or trigger premature dendritic failure remain poorly understood. Here, we investigate a series of π-interactive aromatic alcohols and a cycloaliphatic reference additive and uncover how additive–zinc and additive–additive interactions jointly govern the formation, spatial organization, packing density, and mobility of the additive film. These interfacial dynamics govern Zn<sup>2+</sup>transport, corrosion suppression, and zinc deposition morphology. Phenol, which strikes a balance between adsorption strength and interfacial mobility, forms a thick yet dynamic layer that suppresses hydrogen evolution mediated corrosion while promoting uniform zinc deposition. This leads to excellent cycling stability with nearly 2 Ah cm<sup>−2</sup>cumulative plated capacity in a practically relevant asymmetric configuration at 24% depth of discharge under demanding 4 mA cm<sup>−2</sup>–4 mAh cm<sup>−2</sup>, including a thin separator and low electrolyte-to-capacity ratio, with the coulombic efficiency reaching 99.89% under kinetic control compared to 95.94% for the additive-free electrolyte. Full cell and pouch-cell tests further validate phenol's efficacy, establishing adsorption layer dynamics as a new paradigm for rationalizing electrolyte additives’ efficacy in regulating zinc anode reversibility in aqueous batteries.
dc.language	en
dc.publisher	Royal Society of Chemistry (RSC)
dc.relation.ispartof	Energy and Environmental Science
dc.relation.isbasedon	10.1039/d5ee05206h
dc.rights	info:eu-repo/semantics/openAccess
dc.subject.classification	Energy
dc.title	A π-interactive additive unlocks enhanced zinc anode rechargeability: unveiling the critical role of adsorption layer dynamics
dc.type	Journal Article
utslib.citation.volume	18
utslib.copyright.status	open_access	*
dc.rights.license	This work is licensed under a Creative Commons Attribution-NonCommercial 3.0 International License (CC BY-NC 3.0). To view a copy of this license, visit https://creativecommons.org/licenses/by-nc/3.0/
dc.date.updated	2026-05-19T05:15:50Z
pubs.issue	24
pubs.publication-status	Published
pubs.volume	18
utslib.citation.issue	24

Abstract:

Aqueous zinc-ion batteries are promising for a safe, inexpensive, and sustainable platform for stationary energy storage, but their reversibility remains limited by dendrite and corrosion-mediated failure of the zinc anode. While low-concentration electrolyte additives have emerged as scalable solutions, the mechanistic underpinnings of their interfacial dynamics that dictate whether they enable long-term rechargeability or trigger premature dendritic failure remain poorly understood. Here, we investigate a series of π-interactive aromatic alcohols and a cycloaliphatic reference additive and uncover how additive–zinc and additive–additive interactions jointly govern the formation, spatial organization, packing density, and mobility of the additive film. These interfacial dynamics govern Zn²⁺transport, corrosion suppression, and zinc deposition morphology. Phenol, which strikes a balance between adsorption strength and interfacial mobility, forms a thick yet dynamic layer that suppresses hydrogen evolution mediated corrosion while promoting uniform zinc deposition. This leads to excellent cycling stability with nearly 2 Ah cm⁻²cumulative plated capacity in a practically relevant asymmetric configuration at 24% depth of discharge under demanding 4 mA cm⁻²–4 mAh cm⁻², including a thin separator and low electrolyte-to-capacity ratio, with the coulombic efficiency reaching 99.89% under kinetic control compared to 95.94% for the additive-free electrolyte. Full cell and pouch-cell tests further validate phenol's efficacy, establishing adsorption layer dynamics as a new paradigm for rationalizing electrolyte additives’ efficacy in regulating zinc anode reversibility in aqueous batteries.

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http://hdl.handle.net/10453/195063