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Batteries
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Electrolyte and Electrode Design for Next-Generation Rechargeable Batteries
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Electrolyte and Electrode Design for Next-Generation Rechargeable 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: 10 June 2025 | Viewed by 20018

Special Issue Editor

Dr. Shaokun Chong

E-Mail Website
Guest Editor
Frontiers Science Center for Flexible Electronics, Northwestern Polytechnical University, Xi’an 710072, China
Interests: lithium/sodium/potassium ion batteries; advanced electrode materials; nano-composites; electrochemical mechanism; electrocatalysis

Special Issue Information

Dear Colleagues,

Designing qualified electrolytes and electrodes is key to the success of emerging battery systems. Electrode materials play an important role in the energy density, power density, and cycling life of batteries, and the design of reasonable electrode materials is essential to promote the development of novel battery technologies. As the only component that interfaces with every other component in the batteries, the electrolyte must simultaneously satisfy several criteria, including rapid ion and mass transportation, effective electron insulation, and electrochemical inertness. The associated electrolyte–electrode interfacing chemistry is the essence of electrolyte engineering, dictating the power, energy, and reversibility of the battery during its entire service life. This Special Issue will cover the key topics in next-generation “beyond Li-ion” battery technologies, including electrolytes, electrodes, and interphases.

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

  • Novel battery systems;
  • Novel anode and cathode materials;
  • Li/Na/K/Zn metal anode;
  • Catalysts design for electrolytic water systems, fuel cells, Li-O2 batteries, etc.;
  • Electrolyte adjustment;
  • All-solid-state electrolyte design and batteries;
  • Solid electrolyte interface;
  • Electrochemical principles;
  • Failure mechanism of batteries.
  • Full batteries.

Dr. Shaokun Chong
Guest Editor

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

  • rechargeable batteries
  • sodium-ion batteries
  • potassium-ion batteries
  • lithium-ion batteries
  • Li-S batteries
  • Li-O2 batteries
  • electrocatalysis
  • Zn/Mg-ion batteries
  • electrode materials
  • electrolyte engineering
  • electrochemical mechanism
  • electrochemical performances

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Published Papers (10 papers)

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Research

14 pages, 3683 KiB  
Article
Monodisperse Hierarchical N-Doped Carbon Microspheres with Uniform Pores as a Cathode Host for Advanced K–Se Batteries
by Hyun-Jin Kim, Jeong-Ho Na and Seung-Keun Park
Batteries 2025, 11(3), 101; https://doi.org/10.3390/batteries11030101 - 7 Mar 2025
Viewed by 693
Abstract
K–Se batteries offer high energy density and cost-effectiveness, making them promising candidates for energy storage systems. However, their practical applications are hindered by Se aggregation, sluggish ion diffusion, and significant volumetric expansion. To address these challenges, monodisperse hierarchical N-doped carbon microspheres (NCHS) with [...] Read more.
K–Se batteries offer high energy density and cost-effectiveness, making them promising candidates for energy storage systems. However, their practical applications are hindered by Se aggregation, sluggish ion diffusion, and significant volumetric expansion. To address these challenges, monodisperse hierarchical N-doped carbon microspheres (NCHS) with uniformly sized pores were synthesized as cathode hosts. The flower-like microstructure, formed by the assembly of two-dimensional building blocks, mitigated Se aggregation and facilitated uniform distribution within the pores, enhancing Se utilization. Nitrogen doping, introduced during synthesis, strengthened chemical bonding between selenium and the carbon host, suppressed side reactions, and accelerated reaction kinetics. These synergistic effects enabled efficient ion transport, improved electrolyte accessibility, and enhanced redox reactions. Additionally, the uniform particle and pore sizes of NCHS effectively mitigated volumetric expansion and surface accumulation, ensuring long-term cycling stability and superior electrochemical performance. Se-loaded NCHS (Se@NCHS) exhibited a high discharge capacity of 199.4 mA h g−1 at 0.5 C after 500 cycles with 70.4% capacity retention and achieved 188 mA h g−1 at 3.0 C, outperforming conventional carbon hosts such as Super P. This study highlights the significance of structural and chemical modifications in optimizing cathode materials and offers valuable insights for developing high-performance energy storage systems. Full article
(This article belongs to the Special Issue Electrolyte and Electrode Design for Next-Generation Rechargeable Batteries)
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21 pages, 4141 KiB  
Article
Ternary PEO/PVDF-HFP-Based Polymer Electrolytes for Li-Ion Batteries
by Hoang Bao Tran Nguyen, Ling Ding, Björn Pohle, Toni Schmeida, Hoang Bao An Nguyen and Daria Mikhailova
Batteries 2025, 11(2), 45; https://doi.org/10.3390/batteries11020045 - 25 Jan 2025
Viewed by 1561
Abstract
The impetus to study and develop polymer electrolytes for metal-ion batteries is due to their enhanced safety compared to flammable organic liquid electrolytes, promising ionic conductivity, and broad electrochemical stability window, making them to viable candidates for battery application. In the current work, [...] Read more.
The impetus to study and develop polymer electrolytes for metal-ion batteries is due to their enhanced safety compared to flammable organic liquid electrolytes, promising ionic conductivity, and broad electrochemical stability window, making them to viable candidates for battery application. In the current work, we present a simple fabrication procedure and a comprehensive physico–chemical study of various PVDF-HFP-based electrolyte formulations with a sufficient addition of PEO polymer, LiTFSI conducting salt, and EMIMTFSI ionic liquid. The ionic conductivity, activation energy for ionic movement and thickness of the resulting polymer electrolyte show a non-linear dependency on the PVDF-HFP/PEO ratio. The electrolyte composition with a 0.35PEO-0.65PVDF-HFP/1LiTFSI/1EMIMTFSI mass fraction exhibits the highest ionic conductivity among the compositions, revealing 7.7×10−5 S cm−1 at 30 °C. Electrochemical tests in half full and full Li-ion batteries with a LiFePO4 cathode and Li4Ti5O12 anode also emphasized this composition as the most promising one, providing an initial capacity in full cells of 120 mAh g−1 and a capacity retention of about 75% after 50 charge/discharge cycles at a 0.1 C current rate. In the PEO/PVDF-HFP polymer blend with EMIMTFSI as a plasticizer, the amount of crystalline parts, which are detrimental to a fast ionic diffusion, is significantly reduced. Full article
(This article belongs to the Special Issue Electrolyte and Electrode Design for Next-Generation Rechargeable Batteries)
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17 pages, 1931 KiB  
Article
Lithium Tracer Diffusion in LixCoO2 and LixNi1/3Mn1/3Co1/3O2 (x = 1, 0.9, 0.65)-Sintered Bulk Cathode Materials for Lithium-Ion Batteries
by Erwin Hüger, Daniel Uxa and Harald Schmidt
Batteries 2025, 11(2), 40; https://doi.org/10.3390/batteries11020040 - 21 Jan 2025
Viewed by 873
Abstract
The knowledge of Li diffusivities in electrode materials of Li-ion batteries (LIBs) is essential for a fundamental understanding of charging/discharging times, maximum capacities, stress formation and possible side reactions. The literature indicates that Li diffusion in the cathode material Li(Ni,Mn,Co)O2 strongly increases [...] Read more.
The knowledge of Li diffusivities in electrode materials of Li-ion batteries (LIBs) is essential for a fundamental understanding of charging/discharging times, maximum capacities, stress formation and possible side reactions. The literature indicates that Li diffusion in the cathode material Li(Ni,Mn,Co)O2 strongly increases during electrochemical delithiation. Such an increased Li diffusivity will be advantageous for performance if it is present already in the initial state after synthesis. In order to understand the influence of a varying initial Li content on Li diffusion, we performed Li tracer diffusion experiments on LixCoO2 (LCO) and LixNi1/3Mn1/3Co1/3O2 (NMC, x = 1, 0.9, 0.65) cathode materials. The measurements were performed on polycrystalline sintered bulk materials, free of additives and binders, in order to study the intrinsic properties. The variation of Li content was achieved using reactive solid-state synthesis using pressed Li2CO3, NiO, Co3O4 and/or MnO2 powders and high temperature sintering at 800 °C. XRD analyses showed that the resultant bulk samples exhibit the layered LCO or NMC phases with a low amount of cation intermixing. Moreover, the presence of additional NiO and Co3O4 phases was detected in NMC with a pronounced nominal Li deficiency of x = 0.65. As a tracer source, a 6Li tracer layer with the same chemical composition was deposited using ion beam sputtering. Secondary ion mass spectrometry in depth profile mode was used for isotopic analysis. The diffusivities followed the Arrhenius law with an activation enthalpy of about 0.8 eV and were nearly identical within error for all samples investigated in the temperature range up to 500 °C. For a diffusion mechanism based on structural Li vacancies, the results indicated that varying the Li content does not result in a change in the vacancy concentration. Consequently, the design and use of a cathode initially made of a Li-deficient material will not improve the kinetics of battery performance. The possible reasons for this unexpected result are discussed. Full article
(This article belongs to the Special Issue Electrolyte and Electrode Design for Next-Generation Rechargeable Batteries)
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10 pages, 2269 KiB  
Article
Concentrated, Gradient Electrolyte Design for Superior Low-Temperature Li-Metal Batteries
by Jason S. Packard, Ethan A. Adams and Vilas G. Pol
Batteries 2024, 10(12), 448; https://doi.org/10.3390/batteries10120448 - 18 Dec 2024
Viewed by 1043
Abstract
Improving the low-temperature performance of lithium-ion batteries is critical for their widespread adoption in cold environments. In this study, we designed a novel LHCE featuring a solvent polarity gradient, designed to maximize both room- and low-temperature ion mobility. Extremely polar fluoroethylene carbonate (FEC) [...] Read more.
Improving the low-temperature performance of lithium-ion batteries is critical for their widespread adoption in cold environments. In this study, we designed a novel LHCE featuring a solvent polarity gradient, designed to maximize both room- and low-temperature ion mobility. Extremely polar fluoroethylene carbonate (FEC) and low-freezing-point, −135 °C, non-polar nonaflurobutyl methyl ether (NONA) were supplemented by two intermediate solvents with incremental step-downs in polarity. The intermediate solvents consist of methyl (2,2,2-triflooethyl) carbonate (FEMC) and either diethylene carbonate (DEC), ethyl methyl carbonate (EMC), or dibutyl carbonate (DBC). The four solvents were combined with 1 M lithium bis(fluorosulfonyl)amide (LiFSI) salt and were able to accommodate 37.5% diluent volume, resulting in ultra-low electrolyte freezing points below −120 °C. This contrasts with our previously investigated three-solvent LHCE, which only allowed for a 14% diluent volume and a −85 °C freezing point. Localized high salt concentrations were shown by less than 3% of FSI- anions being free in solution. The gradient LHCEs also showed room-temperature ionic conductivities above 10–3 S/cm and maintained high ion mobility below −40 °C. Lithium metal coin cells with LiFePO4 (LFP) cathodes featuring the gradient LHCEs, a reference three-solvent LHCE, and commercial (1 M LiPF6 in 1:1 EC:DEC) electrolyte were constructed. All gradient LHCEs outperformed both the three-solvent and commercial electrolytes at all temperatures, with the DEC-based gradient LHCE showing the best performance of 159.7 mAh/g at 25 °C and 109.2 mAh/g at −50 °C, corresponding to a 68% capacity retention. These findings highlight the potential of LHCE systems to improve battery performance in low-temperature environments and propose a new gradient design strategy for electrolytes to yield advantages of both polar and weakly polar solvents. Full article
(This article belongs to the Special Issue Electrolyte and Electrode Design for Next-Generation Rechargeable Batteries)
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12 pages, 1657 KiB  
Article
Study of Cathode Materials for Na-Ion Batteries: Comparison Between Machine Learning Predictions and Density Functional Theory Calculations
by Claudio Ronchetti, Sara Marchio, Francesco Buonocore, Simone Giusepponi, Sergio Ferlito and Massimo Celino
Batteries 2024, 10(12), 431; https://doi.org/10.3390/batteries10120431 - 5 Dec 2024
Viewed by 1580
Abstract
Energy storage technologies have experienced significant advancements in recent decades, driven by the growing demand for efficient and sustainable energy solutions. The limitations associated with lithium’s supply chain, cost, and safety concerns have prompted the exploration of alternative battery chemistries. For this reason, [...] Read more.
Energy storage technologies have experienced significant advancements in recent decades, driven by the growing demand for efficient and sustainable energy solutions. The limitations associated with lithium’s supply chain, cost, and safety concerns have prompted the exploration of alternative battery chemistries. For this reason, research to replace widespread lithium batteries with sodium-ion batteries has received more and more attention. In the present work, we report cutting-edge research, where we explored a wide range of compositions of cathode materials for Na-ion batteries by first-principles calculations using workflow chains developed within the AiiDA framework. We trained crystal graph convolutional neural networks and geometric crystal graph neural networks, and we demonstrate the ability of the machine learning algorithms to predict the formation energy of the candidate materials as calculated by the density functional theory. This materials discovery approach is disruptive and significantly faster than traditional physics-based computational methods. Full article
(This article belongs to the Special Issue Electrolyte and Electrode Design for Next-Generation Rechargeable Batteries)
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21 pages, 15469 KiB  
Article
Synthesis and Characterization of Lithium Phosphate (Li3PO4) as a Solid Electrolyte
by Seybou Yacouba Zakariyaou, Hua Ye and Chongwen Jiang
Batteries 2024, 10(12), 429; https://doi.org/10.3390/batteries10120429 - 3 Dec 2024
Viewed by 3228
Abstract
Due to its high thermal stability, environmental friendliness, and safety, lithium phosphate (Li3PO4) is used as a solid electrolyte in battery applications, but it is usually used with dopants due to its lower ionic conductivity, which is required for [...] Read more.
Due to its high thermal stability, environmental friendliness, and safety, lithium phosphate (Li3PO4) is used as a solid electrolyte in battery applications, but it is usually used with dopants due to its lower ionic conductivity, which is required for ion transport. However, due to its stability and environmentally friendly aspect, lithium phosphate is still a hot topic among suitable energy materials that need further research to improve its electrochemical properties. In the current work, a novel synthesis of lithium phosphate was proposed from the raw materials lithium carbonate (Li2CO3) and trisodium phosphate dodecahydrate (Na3PO4*12H2O) under suitable stoichiometric conditions using the co-precipitation method. In the set of synthesized samples, a single-phase β-Li3PO4 (named LPO-4) with 99.7% purity and 93.49% yield was successfully prepared under appropriate stoichiometric conditions and pH 13 at 90 °C. The average particle size was 10 nm with a large surface area of 9.02 m2g−1. Electrochemical impedance spectroscopy (EIS) of LPO-4 revealed a conductivity of 7.1 × 10−6 S.cm−1 at room temperature and 2.7 × 10−5 S.cm−1 at 80 °C with a low activation energy of 0.38 eV. This performance is attributed to the morphology of the nanotubes and the smaller particle size, which enlarge the reaction interfaces and shorten the diffusion distance of lithium ions. The kinetic and thermodynamic key parameters showed that the β-Li3PO4 exhibits thermal stability in the room temperature range up to 208.8 °C. All these property values indicate a promising application of lithium phosphate as a solid electrolyte in solid-state batteries and a new route for further investigation. Full article
(This article belongs to the Special Issue Electrolyte and Electrode Design for Next-Generation Rechargeable Batteries)
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11 pages, 2929 KiB  
Article
Dendrite-Free Zn Anode Modified by Organic Coating for Stable Aqueous Zinc Ion Batteries
by Fujie Li, Hongfei Zhang, Xuehua Liu, Binghui Xu and Chao Wang
Batteries 2024, 10(12), 420; https://doi.org/10.3390/batteries10120420 - 29 Nov 2024
Viewed by 1326
Abstract
Aqueous zinc-ion batteries (AZIBs) have emerged as highly promising options for large-scale energy storage systems due to their cost-effectiveness, substantial energy capacity, and improved safety features. However, the Zn anode faces challenges such as self-corrosion and dendrite formation, which limit its practical use [...] Read more.
Aqueous zinc-ion batteries (AZIBs) have emerged as highly promising options for large-scale energy storage systems due to their cost-effectiveness, substantial energy capacity, and improved safety features. However, the Zn anode faces challenges such as self-corrosion and dendrite formation, which limit its practical use in AZIB applications. In this work, a simple blade-coating method was used to successfully coat poly (vinylidene fluoride–hexafluoro propylene) (PVDF-HFP) on the Zn anode. The coated Zn anode (P-Zn) displayed a stable cycling performance (700 h) at 1 mA cm−2 current density in the symmetric cell. In addition, the full cell using MnO2 as the cathode and P-Zn as the anode retained almost full capacity even after 1400 cycles at 2C, far outperforming the full cell using the unmodified Zn anode with only 50% capacity retention after 600 cycles. In situ optical observations of Zn deposition demonstrate that the special organic coating significantly enhances the uniform deposition of Zn2+, thus effectively mitigating corrosion and hydrogen evolution. Density Functional Theory (DFT) calculations show that the PVDF-HFP coating effectively narrows the adsorption energy gap between the P-Zn (002) and (101) planes, leading to the homogeneous deposition of Zn2+ with fewer Zn dendrites. A simple and feasible strategy for designing ultra-stable AZIBs by coating an organic protective layer on the Zn surface is provided by this work. Full article
(This article belongs to the Special Issue Electrolyte and Electrode Design for Next-Generation Rechargeable Batteries)
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9 pages, 5523 KiB  
Article
Gravure-Printed Anodes Based on Hard Carbon for Sodium-Ion Batteries
by Maria Montanino, Claudia Paoletti, Anna De Girolamo Del Mauro and Giuliano Sico
Batteries 2024, 10(11), 407; https://doi.org/10.3390/batteries10110407 - 20 Nov 2024
Viewed by 1117
Abstract
Printed batteries are increasingly being investigated for feeding small, wearable devices more and more involved in our daily lives, promoting the study of printing technologies. Among these, gravure is very attractive as a low-cost and low-waste production method for functional layers in different [...] Read more.
Printed batteries are increasingly being investigated for feeding small, wearable devices more and more involved in our daily lives, promoting the study of printing technologies. Among these, gravure is very attractive as a low-cost and low-waste production method for functional layers in different fields, such as energy, sensors, and biomedical, because it is easy to scale up industrially. Thanks to our research, the feasibility of gravure printing was recently proved for rechargeable lithium-ion batteries (LiBs) manufacturing. Such studies allowed the production of high-quality electrodes involving different active materials with high stability, reproducibility, and good performance. Going beyond lithium-based storage devices, our attention was devoted on the possibility of employing highly sustainable gravure printing for sodium-ion batteries (NaBs) manufacturing, following the trendy interest in sodium, which is more abundant, economical, and ecofriendly than lithium. Here a study on gravure printed anodes for sodium-ion batteries based on hard carbon as an active material is presented and discussed. Thanks to our methodology centered on the capillary number, a high printing quality anodic layer was produced providing typical electrochemical behavior and good performance. Such results are very innovative and relevant in the field of sodium-ion batteries and further demonstrate the high potential of gravure in printed battery manufacturing. Full article
(This article belongs to the Special Issue Electrolyte and Electrode Design for Next-Generation Rechargeable Batteries)
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23 pages, 5711 KiB  
Article
Deciphering Electrolyte Degradation in Sodium-Based Batteries: The Role of Conductive Salt Source, Additives, and Storage Condition
by Mahir Hashimov and Andreas Hofmann
Batteries 2023, 9(11), 530; https://doi.org/10.3390/batteries9110530 - 25 Oct 2023
Cited by 8 | Viewed by 4538
Abstract
This work investigates the stability of electrolyte systems used in sodium-ion-based batteries. The electrolytes consist of a 1:1 (v:v) mixture of ethylene carbonate (EC) and propylene carbonate (PC), a sodium-conducting salt (either NaPF6 or NaTFSI), and fluoroethylene carbonate [...] Read more.
This work investigates the stability of electrolyte systems used in sodium-ion-based batteries. The electrolytes consist of a 1:1 (v:v) mixture of ethylene carbonate (EC) and propylene carbonate (PC), a sodium-conducting salt (either NaPF6 or NaTFSI), and fluoroethylene carbonate (FEC), respectively, sodium difluoro(oxalato) borate (NaDFOB), as additives. Through systematic evaluation using gas chromatography coupled with mass spectrometry (GC-MS), we analyze the formation of degradation products under different conditions including variations in temperature, vial material, and the presence or absence of sodium metal. Our results reveal the significant influence of the conductive salt’s source on degradation. Furthermore, we observe that FEC’s stability is affected by the storage temperature, vial material, and presence of sodium metal, suggesting its active involvement in the degradation process. Additionally, our results highlight the role of NaDFOB as an additive in mitigating degradation. The study provides crucial insights into the complex network of degradation reactions occurring within the electrolyte, thus informing strategies for improved electrolyte systems in sodium-based batteries. Since the production, material selection and storage of electrolytes are often insufficiently described, we provide here an insight into the different behavior of electrolytes for Na-ion batteries. Full article
(This article belongs to the Special Issue Electrolyte and Electrode Design for Next-Generation Rechargeable Batteries)
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12 pages, 4782 KiB  
Article
Bismuth Nano-Rods Wrapped with Graphene and N-Doped C as Anode Materials for Potassium- and Sodium-Ion Batteries
by Shuangyan Qiao, Yongning Liu, Kai Wang and Shaokun Chong
Batteries 2023, 9(10), 505; https://doi.org/10.3390/batteries9100505 - 4 Oct 2023
Cited by 8 | Viewed by 2621
Abstract
Alloying-type anode materials have considerably promoted the development of potassium-ion batteries (PIBs) and sodium-ion batteries (SIBs), enabling them to achieve high-energy-density. However, large volume expansion and sluggish dynamic behavior have become key issues affecting electrochemical performance. Herein, bismuth (Bi) nano-rods are anchored on [...] Read more.
Alloying-type anode materials have considerably promoted the development of potassium-ion batteries (PIBs) and sodium-ion batteries (SIBs), enabling them to achieve high-energy-density. However, large volume expansion and sluggish dynamic behavior have become key issues affecting electrochemical performance. Herein, bismuth (Bi) nano-rods are anchored on reduced graphene (rGO) and encapsulated via N-doped C (NC) to construct Bi@rGO@NC architecture as anode materials for SIBs and PIBs. The hierarchical confinement effect of three-dimensional conductive networks can not only improve electrode stability upon cycling via suppressing the large volume variation, but also eliminate the band gap of Bi and accelerate ion diffusion, thereby exhibiting favorable electrochemical reaction kinetics. Thus, Bi@rGO@NC contributes an ultra-long lifetime, over 1000 cycles, and an outstanding rate property to SIBs and PIBs. This work can pave the way for the construction of high-performance alloying-type anode materials for SIBs and PIBs. Full article
(This article belongs to the Special Issue Electrolyte and Electrode Design for Next-Generation Rechargeable Batteries)
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