journal article·2025-11-14

Bilateral Helmholtz Plane Tailoring in Low-Concentration Electrolytes for Practical Zinc–Vanadium Batteries

Jian Qin, Tianshuai Wang, Minhao Dai, Na Wu, Shuai Chen, Xiujuan Zhang, Xifei Li, Jiansheng Jie

ACS Energy Letters· Volume 10· Issue 11
Publisher page

Abstract

Vanadium-based zinc-ion batteries (ZIBs) fail due to electrolyte concentration-dependent bilateral instabilities at the inner Helmholtz plane (IHP). This work demonstrates bilateral IHP tailoring that unlocks stable battery operation in low-concentration electrolytes. Cathodically, a compact AN-derived adlayer suppresses V–OH deprotonation and induces charge reversal, while electrostatic and spatial effects inhibit proton-triggered vanadium dissolution/shuttling. Anodically, acetonitrile (AN) facilitates Zn 2+ -OTf – contact ion pair formation, inducing in situ generation of a hydrophobic/zincophilic solid electrolyte interphase. Coupled with its selective adsorption on Zn metal and suppression of water activity, this system blocks interfacial H + /H 2 O accumulation, enabling instantaneous Zn nucleation and dendrite-free (002)-oriented deposition. Consequently, the Zn//NVO coin cells exhibit 10000 cycle longevity with 82% capacity retention over the initial 3000 cycles. Practical Zn//VO 2 pouch cells sustain 1200 cycles with high cumulative capacity exceeding 550 Ah, surpassing prior benchmarks. This work establishes a universal bilateral IHP tailoring framework toward cost-effective, durable ZIBs.
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Research context

OpenAlex topics: Advanced battery technologies research · Advanced Battery Materials and Technologies · Advanced Battery Technologies Research

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Macau Institute of Materials Science and Engineering, MUST-SUDA Joint Research Center for Advanced Functional Materials

Macau University of Science and Technology

Institute of Advanced Electrochemical Energy & School of Materials Science and Engineering

Xi’an University of Technology

Xi’an Key Laboratory of Functional Organic Porous Materials, School of Chemistry and Chemical Engineering

Northwestern Polytechnical University

Chongqing Science and Technology Innovation Center of Northwestern Polytechnical University

Institute of Functional Nano & Soft Materials (FUNSOM), State Key Laboratory of Bioinspired Interfacial Materials Science

Soochow University

Funding

Natural Science Foundation of Chongqing Municipality · Natural Science Basic Research Program of Shaanxi Province · National Natural Science Foundation of China · The Science and Technology Development Fund (FDCT) of the Macao Special Administrative Region · Macao Young Scholars Program · Youth Innovation Team Project of Shaanxi Provincial Department of Education

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