Solid Polymer Electrolytes for Lithium Batteries and Beyond

A special issue of Batteries (ISSN 2313-0105). This special issue belongs to the section "Electrolyte and Interfacial Engineering".

Deadline for manuscript submissions: 15 October 2026 | Viewed by 3865

Special Issue Editors


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Guest Editor
Interdisciplinary Science and Engineering Laboratory, Department of Plant and Soil Sciences, University of Delaware, Newark, DE 19716, USA
Interests: sustainable materials; material characterization; surface analysis

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Guest Editor
Electromobility Research Centre (MOBI), Vrije Universiteit Brussel, Pleinlaan 2, 1050 Brussels, Belgium
Interests: lithium-ion battery manufacturing; solid-state Li-ion battery; Ag/ZnO nanocomposite particles; material characterization; materials; nanomaterials; nanomaterials synthesis; materials processing; nanostructured materials; nanoparticle synthesis; ceramics; ceramic materials; battery
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Special Issue Information

Dear Colleagues,

Research on solid polymer electrolytes (SPEs), which seeks to overcome the limitations of conventional liquid electrolytes, has emerged as an important frontier in energy storage technology. These materials eliminate the safety concerns associated with flammable organic solvents while also enabling next-generation battery design, including flexible devices. The growing demand for high-energy-density, safe, and sustainable energy storage solutions has intensified research of SPEs, particularly for lithium-ion batteries and emerging technologies like lithium metal batteries, sodium-ion, and multivalent-ion systems.

This Special Issue aims to disseminate the most recent advances in solid polymer electrolyte research, covering fundamental science, materials development, upscaling, and technological applications through both original research outputs and comprehensive reviews of the state of the art.

Areas of interest may include, but are not limited to, the following topics:

  • Novel polymer electrolyte design strategies;
  • Polymer electrolytes with smart functionalities including self-healing;
  • Ion transport mechanisms and conductivity enhancement;
  • Polymer–ceramic composite electrolytes;
  • Interface engineering and electrode compatibility;
  • Mechanical properties and processability;
  • Thermal stability and safety characteristics;
  • Beyond lithium—sodium and multivalent systems;
  • Advanced characterization techniques;
  • Computational modelling and simulation;
  • Manufacturing and scalability considerations;
  • Post-mortem analysis and failure mechanisms in polymer electrolyte systems;
  • Research on scalability and large-scale solid-state battery manufacturing.

Research on solid-state batteries that have at least one compound as polymer (e.g., polymer–ceramic composite electrolyte or gel electrolytes) is highly encouraged. Fuel cell applications, especially with polymer electrolyte fuel cells, and research on polymer compounds in flow batteries are considered to be beyond the scope of this Special Issue.

Dr. Pavlo Ivanchenko
Dr. Kamil Burak Dermenci
Guest Editors

Manuscript Submission Information

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Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Batteries is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • solid polymer electrolytes
  • solid-state batteries
  • lithium batteries
  • ion conductivity
  • polymer–ceramic composites
  • interface engineering
  • electrolyte design
  • battery safety
  • beyond lithium systems
  • energy storage materials

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Published Papers (3 papers)

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Research

23 pages, 3712 KB  
Article
Nitrogen-Enriched Shell Graphite-Core C–Si–N Composite for Reduced Swelling in Si/Graphite Negative Electrodes
by Jeewon Jang, Seongwoo Lee, Sangyup Lee, Paul Maldonado Nogales, Honggeun Lee, Seunga Yang, Minji Kim, Jeonghun Oh and Soon-Ki Jeong
Batteries 2026, 12(3), 98; https://doi.org/10.3390/batteries12030098 - 13 Mar 2026
Viewed by 754
Abstract
This study reports a graphite-core, multiphase gradient C–Si–N composite architecture for Si-containing graphite-based negative electrodes in lithium-ion batteries. The increase in electrode thickness is used as a practical metric of expansion-driven degradation. The composite is prepared by the simultaneous nitridation and carbonization of [...] Read more.
This study reports a graphite-core, multiphase gradient C–Si–N composite architecture for Si-containing graphite-based negative electrodes in lithium-ion batteries. The increase in electrode thickness is used as a practical metric of expansion-driven degradation. The composite is prepared by the simultaneous nitridation and carbonization of a graphite core–Si precursor using polyvinylpyrrolidone (PVP) as the N source. Scanning electron microscopy coupled with energy-dispersive X-ray spectroscopy indicates a quasi-continuous radial trend in the relative N signal toward the outer shell, consistent with preferential N enrichment near the particle exterior. This spatially distributed N arrangement may spatially separate the Si-rich expansion-prone region from the carbon-rich exterior containing nitrides and other N-bearing species, thereby enabling stress partitioning. The shell architecture is designed to disperse expansion-induced stress and stabilize the electrode–electrolyte interface. During electrochemical cycling, the C–Si–N electrode with 10% PVP preserves its core–shell morphology and exhibits the smallest average electrode thickness expansion (~58% after 40 cycles, based on four independent cells). The reduced thickness growth is discussed in relation to a mechanically robust Si–N matrix (Si3N4-like/SiNx-like), potential Li–N interphase species, and N-containing carbon, together with the post-mortem morphology and electrochemical impedance evolution. This study presents reduced swelling as an electrode-level trend versus nominal PVP addition, along with associated nitride-related signatures, thereby highlighting spatially graded stress buffering as an electrode-level design principle. Full article
(This article belongs to the Special Issue Solid Polymer Electrolytes for Lithium Batteries and Beyond)
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16 pages, 6964 KB  
Article
Application of Li3InCl6-PEO Composite Electrolyte in All-Solid-State Battery
by Han-Xin Mei, Paolo Piccardo and Roberto Spotorno
Batteries 2026, 12(1), 21; https://doi.org/10.3390/batteries12010021 - 6 Jan 2026
Viewed by 1558
Abstract
Poly(ethylene oxide) (PEO)-based solid polymer electrolytes typically suffer from limited ionic conductivity at near-room temperature and often require inorganic reinforcement. Halide solid-state electrolytes such as Li3InCl6 (LIC) offer fast Li+ transport but are moisture-sensitive and typically require pressure-assisted densification. [...] Read more.
Poly(ethylene oxide) (PEO)-based solid polymer electrolytes typically suffer from limited ionic conductivity at near-room temperature and often require inorganic reinforcement. Halide solid-state electrolytes such as Li3InCl6 (LIC) offer fast Li+ transport but are moisture-sensitive and typically require pressure-assisted densification. Here, we fabricate a flexible LIC–PEO composite electrolyte via slurry casting in acetonitrile with a small amount of LiPF6 additive. The free-standing membrane delivers an ionic conductivity of 1.19 mS cm−1 at 35 °C and an electrochemical stability window up to 5.15 V. Compared with pristine LIC, the composite shows improved moisture tolerance, and its conductivity can be recovered by mild heating after exposure. The electrolyte enables stable Li|LIC–PEO|Li cycling for >620 h and supports Li|LIC–PEO|NCM111 cells with capacity retentions of 84.2% after 300 cycles at 0.2 C and 80.6% after 150 cycles at 1.2 C (35 °C). Structural and surface analyses (XRD, SEM/EDX, XPS) elucidate the composite microstructure and interfacial chemistry. Full article
(This article belongs to the Special Issue Solid Polymer Electrolytes for Lithium Batteries and Beyond)
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19 pages, 3215 KB  
Article
Thick LiMn2O4 Electrode with Polymer Electrolyte for Electrochemical Extraction of Lithium from Brines
by Daiwei Yao, Jing Qin, Hongtan Liu, Mert Akin and Xiangyang Zhou
Batteries 2025, 11(12), 454; https://doi.org/10.3390/batteries11120454 - 10 Dec 2025
Cited by 1 | Viewed by 986
Abstract
Thick (900–1500 µm), crack-free lithium manganese oxide (LMO) electrodes with a polyvinylidene fluoride (PVDF)-based polymer electrolyte were prepared using an innovated slurry casting method. The selectivity and intercalation capacity of the thick electrodes of 900–1500 μm were evaluated in aqueous chloride solutions containing [...] Read more.
Thick (900–1500 µm), crack-free lithium manganese oxide (LMO) electrodes with a polyvinylidene fluoride (PVDF)-based polymer electrolyte were prepared using an innovated slurry casting method. The selectivity and intercalation capacity of the thick electrodes of 900–1500 μm were evaluated in aqueous chloride solutions containing main cations in synthetic Salar de Atacama brine using cyclic voltammetry (CV) measurements. The CV data indicated that a high Li+ selectivity of Li/Na = 152.7 could be achieved under potentiostatic conditions. With the thickest electrode, while the mass specific intercalation capacity was 6.234 mg per gram of LMO, the area specific capacity was increased by 3–11 folds compared to that for conventional thin electrodes to 0.282 mg per square centimeter. In addition, 82% of capacity was retained over 30 intercalation/dis-intercalation cycles. XRD and electrochemical analyses revealed that both Faradaic diffusion-controlled or battery-like intercalation and Faradaic non-diffusion controlled or pseudocapacitive intercalation contributed to the capacity and selectivity. This work demonstrates a practical technology for thick electrode fabrication that promises to result in a significant reduction in manufacturing and operational costs for lithium extraction from brines. Full article
(This article belongs to the Special Issue Solid Polymer Electrolytes for Lithium Batteries and Beyond)
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