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Batteries
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Energy-Dense Metal–Sulfur Batteries
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Energy-Dense Metal–Sulfur Batteries

A special issue of Batteries (ISSN 2313-0105). This special issue belongs to the section "Battery Materials and Interfaces: Anode, Cathode, Separators and Electrolytes or Others".

Deadline for manuscript submissions: closed (10 April 2025) | Viewed by 6205

Special Issue Editors

Dr. Daiwei Wang

E-Mail Website
Guest Editor
Department of Mechanical Engineering, The Pennsylvania State University, University Park, PA 16801, USA
Interests: lithium–sulfur batteries; lithium-ion batteries; solid-state batteries
Dr. Meng Liao

E-Mail Website
Guest Editor
Department of Mechanical Engineering, The Pennsylvania State University, University Park, PA 16801, USA
Interests: lithium–sulfur batteries; batteries; polymeric sulfur cathodes; carbon nanotube; flexible electronics
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Elemental sulfur, with its high theoretical capacity (1675 mAh g−1) and low cost, is among the most promising cathode materials for next-generation battery technologies for use in electric vehicles and stationary energy storage. However, the issue of polysulfide dissolution significantly limits both the energy density and cycle life of metal-sulfur batteries (e.g., Li–S and Na–S batteries). Novel strategies are urgently needed to tackle this challenge. Additionally, the use of all-solid-state metal–sulfur batteries, which eliminate polysulfide dissolution, has recently gained attention as a promising solution. Despite this, the degradation mechanisms—particularly the mechanochemical evolution within the cell—remain poorly understood.

In this Special Issue, we are looking for contributions that

  • Develop conductive hosts to mediate polysulfide dissolution and migration;
  • Synthesize polymeric sulfur active materials with restricted polysulfide dissolution;
  • Promote conversion reaction kinetics using electrocatalysts or electrolyte additives;
  • Fabricate metal–sulfur cells with high mass loading and a low electrolyte-to-sulfur ratio;
  • Develop new liquid/semi-solid/solid-state electrolytes to restrict or fundamentally prevent polysulfide dissolution;
  • Understand the mechanical or chemical evolution of all-solid-state metal–sulfur batteries;
  • Study degradation mechanisms by simulating the evolution of cells or cell components.

Topics of interest include, but are not limited to, the following:

  • Advanced conductive hosts;
  • Structured electrodes;
  • Electrocatalysis of sulfur conversion reactions;
  • Liquid/semi-solid/solid-state electrolyte engineering;
  • Mechanochemical evolutions；
  • Degradation mechanisms.

Dr. Daiwei Wang
Dr. Meng Liao
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

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

  • metal–sulfur battery
  • polysulfide dissolution
  • shuttle effect
  • electrocatalysis
  • electrolyte engineering
  • polymeric sulfur
  • high energy density
  • mechanochemical evolution

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Published Papers (4 papers)

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Research

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13 pages, 890 KiB  
Article
A Reduced-Order Model of Lithium–Sulfur Battery Discharge
by Noushin Haddad and Hosam K. Fathy
Batteries 2025, 11(1), 15; https://doi.org/10.3390/batteries11010015 - 2 Jan 2025
Viewed by 912
Abstract
This paper examines the problem of modeling lithium–sulfur (Li-S) battery discharge dynamics. The importance of this problem stems from the attractive specific energy levels achievable by Li-S batteries, which can be particularly appealing for applications such as aviation electrification. Previous research presents different [...] Read more.
This paper examines the problem of modeling lithium–sulfur (Li-S) battery discharge dynamics. The importance of this problem stems from the attractive specific energy levels achievable by Li-S batteries, which can be particularly appealing for applications such as aviation electrification. Previous research presents different Li-S battery models, including “zero-dimensional” models that neglect diffusion while using the laws of electrochemistry to represent reduction–oxidation (redox) rates. Zero-dimensional models typically succeed in capturing key features of Li-S battery discharge, including the high plateau, low plateau, and dip point visible in the discharge curves of certain Li-S battery chemistries. However, these models’ use of one state variable to represent the mass of each active species tends to furnish high-order models, with many state variables. This increases the computational complexity of model-based estimation and optimal control. The main contribution of this paper is to develop low-order state-space model of Li-S battery discharge. Specifically, the paper starts with a seventh-order zero-dimensional model of Li-S discharge dynamics, analyzes its discharge behavior, constructs phenomenological second- and third-order models capable of replicating this behavior, and parameterizes these models. The proposed models succeed in capturing battery discharge behavior accurately over a wide range of discharge rates. To the best of our knowledge, these are two of the simplest published models capable of doing so. Full article
(This article belongs to the Special Issue Energy-Dense Metal–Sulfur Batteries)
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12 pages, 3498 KiB  
Article
An Integrated Na2S−Electrocatalyst Nanostructured Cathode for Sodium–Sulfur Batteries at Room Temperature
by Sichang Ma, Yueming Zhu, Yadong Yang, Dongyang Li, Wendong Tan, Ling Gao, Wanwei Zhao, Wenbo Liu, Wenyu Liang and Rui Xu
Batteries 2025, 11(1), 9; https://doi.org/10.3390/batteries11010009 - 27 Dec 2024
Viewed by 947
Abstract
Room-temperature sodium–sulfur (RT Na–S) batteries offer a superior, high-energy-density solution for rechargeable batteries using earth-abundant materials. However, conventional RT Na–S batteries typically use sulfur as the cathode, which suffers from severe volume expansion and requires pairing with a sodium metal anode, raising significant [...] Read more.
Room-temperature sodium–sulfur (RT Na–S) batteries offer a superior, high-energy-density solution for rechargeable batteries using earth-abundant materials. However, conventional RT Na–S batteries typically use sulfur as the cathode, which suffers from severe volume expansion and requires pairing with a sodium metal anode, raising significant safety concerns. Utilizing Na2S as the cathode material addresses these issues, yet challenges such as Na2S’s low conductivity as well as the shuttle effect of polysulfide still hinder RT Na–S battery development. Herein, we present a simple and cost-effective method to fabricate a Na2S–Na6CoS4/Co@C cathode, wherein Na2S nanoparticles are embedded in a conductive carbon matrix and coupled with dual catalysts, Na6CoS4 and Co, generated via the in situ carbothermal reduction of Na2SO4 and CoSO4. This approach creates a three-dimensional porous composite cathode structure that facilitates electrolyte infiltration and forms a continuous conductive network for efficient electron transport. The in situ formed Na6CoS4/Co electrocatalysts, tightly integrated with Na2S, exhibit strong catalytic activity and robust physicochemical stabilization, thereby accelerating redox kinetics and mitigating the polysulfide shuttle effect. As a result, the Na2S–Na6CoS4/Co@C cathode achieves superior capacity retention, demonstrating a discharge capacity of 346 mAh g−1 after 100 cycles. This work highlights an effective strategy for enhancing Na2S cathodes with embedded catalysts, leading to enhanced reaction kinetics and superior cycling stability. Full article
(This article belongs to the Special Issue Energy-Dense Metal–Sulfur Batteries)
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14 pages, 3115 KiB  
Article
Addition of a Polar, Porous Phase-Inversion-PVDF Membrane to Lithium–Sulfur Cells (LSBs) Already with a Microporous Polypropylene Separator Enhances the Battery Performance
by Irshad Mohammad, Luke D. J. Barter, Carol Crean and Robert C. T. Slade
Batteries 2024, 10(8), 293; https://doi.org/10.3390/batteries10080293 - 21 Aug 2024
Viewed by 2129
Abstract
Lithium–sulfur batteries (LSBs) are widely studied as an alternative to lithium-ion batteries, this emphasis being due to their high theoretical energy density and low cost, and to the high natural abundance of sulfur. Lithium polysulfide shuttling and lithium dendrite growth have limited their [...] Read more.
Lithium–sulfur batteries (LSBs) are widely studied as an alternative to lithium-ion batteries, this emphasis being due to their high theoretical energy density and low cost, and to the high natural abundance of sulfur. Lithium polysulfide shuttling and lithium dendrite growth have limited their commercialization. Porous polyvinylidene fluoride (PVDF) separators have shown improved performance (relative to hydrocarbon separators) in lithium-ion batteries due to faster lithium-ion migration and higher Li+ transference number. A thin polar PVDF membrane has now been fabricated via phase inversion (an immersion-precipitation method) yielding a β (polar) phase concentration of 72%. Preparation from commercial PVDF used dimethylformamide (DMF) solvent at the optimized crystallizing temperature of 70 °C, and pores in the membrane were generated by exchange of DMF with deionized water as non-solvent. The polar PVDF film produced has the advantages of being ultrathin (15 µm), lightweight (1.15 mg cm−2), of high porosity (75%) and high wettability (84%), and it shows enhanced thermal stability relative to polypropylene (PP). The porous, polar PVDF membrane was combined with a commercially available PP membrane to give a hybrid, two-layer, separator combination for LSBs. A synergy was created in the two-layer separator, providing high sulfur utilization and curbing polysulfide shuttling. The electrochemical performance with the hybrid separator (PP–β-PVDF) was evaluated in LSB cells and showed good cyclability and rate capability: those LSB cells showed a stable capacity of 750 mA h g−1 after 100 cycles at 0.1 C, much higher than that for otherwise-identical cells using a commercial PP-only separator (480 mA h g−1). Full article
(This article belongs to the Special Issue Energy-Dense Metal–Sulfur Batteries)
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Review

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25 pages, 8396 KiB  
Review
A Review of Lithium–Sulfur Batteries Based on Metal–Organic Frameworks: Progress and Prospects
by Qiancheng Zhu, Weize Sun, Hua Zhou and Deyu Mao
Batteries 2025, 11(3), 89; https://doi.org/10.3390/batteries11030089 - 22 Feb 2025
Cited by 1 | Viewed by 1443
Abstract
Lithium–sulfur batteries (LSBs) are considered candidates for next-generation energy storage systems due to their high theoretical energy density and low cost. However, their practical applications are constrained by the shuttle effect, lithium dendrites, low conductivity, and volume expansion of sulfur. Metal–organic frameworks (MOFs) [...] Read more.
Lithium–sulfur batteries (LSBs) are considered candidates for next-generation energy storage systems due to their high theoretical energy density and low cost. However, their practical applications are constrained by the shuttle effect, lithium dendrites, low conductivity, and volume expansion of sulfur. Metal–organic frameworks (MOFs) have emerged as promising materials for addressing these challenges, owing to their exceptional adsorption and catalysis capabilities, coupled with a readily adjustable form-factor design. This review provides a broader perspective by comprehensively examining the applications of MOFs in LSBs, covering their roles in cathodes, separators, and electrolytes from multiple dimensions, including their reaction mechanisms, the development potential of MOFs as cathode materials, and the positive impacts on LSBs’ performance achieved through the preparation of MOFs and modifications of intermediate, separator, and electrolyte. Finally, we provide perspectives on future development directions in this field. Full article
(This article belongs to the Special Issue Energy-Dense Metal–Sulfur Batteries)
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