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Solid State Batteries: From Materials Research to Design and Applications

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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 (31 December 2023) | Viewed by 30329

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Special Issue Editors

Prof. Dr. Chunwen Sun

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Guest Editor

School of Chemical and Environmental Engineering, China University of Mining & Technology (Beijing), Beijing 100083, China
Interests: energy storage materials and technologies (all-solid-state batteries, Li/Na-ion batteries, aluminum-ion batteries; fuel cells (solid oxide fuel cells, proton exchange membrane fuel cell catalysts); electrocatalysis (ORR, OER, HER, CO₂ electroreduction); nanomaterials

Prof. Dr. Siqi Shi

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Guest Editor

School of Materials Science and Engineering, Shanghai University, Shanghai 200444, China
Interests: computational materials science; machine learning; electrochemical energy storage materials; ionic transport physics

Dr. Yongjie Zhao

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Guest Editor

School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
Interests: functional ceramic materials; low cost and large-scale preparation of oxide based ceramic electrolyte and its application in solid-state batteries; Na-ion batteries

Special Issue Information

Dear Colleagues,

Solid-state batteries (SIB) with solid electrolytes are considered to be the new generation of devices for energy storage and electric vehicle applications. Is it possible to boost the performance and reduce the cost of solid-state batteries through the rational design of materials, developing key technologies for improving interfacial properties as well as the innovation of manufacturing processes? This Special Issue will cover the key topics in various solid-state batteries.

Topics of interest include, but are not limited to:

Electrode materials for novel solid-state batteries, including positive and negative electrodes;
Solid electrolytes;
Interfacial optimization;
Cell design;
Electrochemical test method;
Cell failure analysis;
Performance lifetime and degradation studies.

Prof. Dr. Chunwen Sun
Prof. Dr. Siqi Shi
Dr. Yongjie Zhao
Guest Editors

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Keywords

solid-state batteries
solid electrolyte
electrode–electrolyte interface
advanced characterization
theory calculation

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Published Papers (10 papers)

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Research

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12 pages, 10472 KiB

Open AccessArticle

Micro-Sized MoS₆@15%Li₇P₃S₁₁ Composite Enables Stable All-Solid-State Battery with High Capacity

by Mingyuan Chang, Mengli Yang, Wenrui Xie, Fuli Tian, Gaozhan Liu, Ping Cui, Tao Wu and Xiayin Yao

Batteries 2023, 9(11), 560; https://doi.org/10.3390/batteries9110560 - 17 Nov 2023

Cited by 2 | Viewed by 2124

Abstract

All-solid-state lithium batteries without any liquid organic electrolytes can realize high energy density while eliminating flammability issues. Active materials with high specific capacity and favorable interfacial contact within the cathode layer are crucial to the realization of good electrochemical performance. Herein, we report a high-capacity polysulfide cathode material, MoS₆@15%Li₇P₃S₁₁, with a particle size of 1–4 μm. The MoS₆ exhibited an impressive initial specific capacity of 913.9 mAh g⁻¹ at 0.1 A g⁻¹. When coupled with the Li₇P₃S₁₁ electrolyte coating layer, the resultant MoS₆@15%Li₇P₃S₁₁ composite showed improved interfacial contact and an optimized ionic diffusivity range from 10⁻¹²–10⁻¹¹ cm² s⁻¹ to 10⁻¹¹–10⁻¹⁰ cm² s⁻¹. The Li/Li₆PS₅Cl/MoS₆@15%Li₇P₃S₁₁ all-solid-state lithium battery delivered ultra-high initial and reversible specific capacities of 1083.8 mAh g⁻¹ and 851.5 mAh g⁻¹, respectively, at a current density of 0.1 A g⁻¹ within 1.0–3.0 V. Even under 1 A g⁻¹, the battery maintained a reversible specific capacity of 400 mAh g⁻¹ after 1000 cycles. This work outlines a promising cathode material with intimate interfacial contact and superior ionic transport kinetics within the cathode layer as well as high specific capacity for use in all-solid-state lithium batteries. Full article

(This article belongs to the Special Issue Solid State Batteries: From Materials Research to Design and Applications)

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12 pages, 11637 KiB

Open AccessArticle

Optimizing Li Ion Transport in a Garnet-Type Solid Electrolyte via a Grain Boundary Design

by Tao Sun, Xiaopeng Cheng, Tianci Cao, Mingming Wang, Jiao Tian, Tengfei Yan, Dechen Qin, Xianqiang Liu, Junxia Lu and Yuefei Zhang

Batteries 2023, 9(11), 526; https://doi.org/10.3390/batteries9110526 - 24 Oct 2023

Cited by 1 | Viewed by 2205

Abstract

Garnet-type solid electrolytes have gained considerable attention owing to their exceptional ionic conductivity and broad electrochemical stability window, making them highly promising for solid-state batteries (SSBs). However, this polycrystalline ceramic electrolyte contains an abundance of grain boundaries (GBs). During the repetitive electroplating and stripping of Li ions, uncontrolled growth and spreading of lithium dendrites often occur at GBs, posing safety concerns and resulting in a shortened cycle life. Reducing the formation and growth of lithium dendrites can be achieved by rational grain boundary design. Herein, the garnet-type solid electrolyte LLZTO was firstly coated with Al₂O₃ using the atomic layer deposition (ALD) technique. Subsequently, an annealing treatment was employed to introduce Al₂O₃ into grain boundaries, effectively modifying them. Compared with the Li/LLZTO/Li cells, the Li/LLZTO@Al₂O₃-annealed/Li symmetric batteries exhibit a more stable cycling performance with an extended period of 200 h at 1 mA cm⁻². After matching with the NMC811 cathode, the capacity retention rate of batteries can reach 96.8% after 50 cycles. The infusion of Al₂O₃ demonstrates its capability to react with LLZTO particles, creating an ion-conducting interfacial layer of Li-Al-O at the GBs. This interfacial layer effectively inhibits Li nucleation and filament growth within LLZTO, contributing to the suppression of lithium dendrites. Our work provides new suggestions for optimizing the synthesis of solid-state electrolytes, which can help facilitate the commercial application of solid-state batteries. Full article

(This article belongs to the Special Issue Solid State Batteries: From Materials Research to Design and Applications)

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12 pages, 4323 KiB

Open AccessArticle

Effect of Carrier Film Phase Conversion Time on Polyacrylate Polymer Electrolyte Properties in All-Solid-State LIBs

by Shujian Zhang, Hongmo Zhu, Lanfang Que, Xuning Leng, Lei Zhao and Zhenbo Wang

Batteries 2023, 9(9), 471; https://doi.org/10.3390/batteries9090471 - 19 Sep 2023

Viewed by 1497

Abstract

To optimize the preparation process of polymer electrolytes by in situ UV curing and improve the performance of polymer electrolytes, we investigated the effect of carrier film phase conversion time on the properties of polymer electrolyte properties in all-solid-state LIBs. We compared several carrier films with phase conversion times of 24 h, 32 h, 40 h, and 48 h. Then, the physical properties of the polymer electrolytes were characterized and the properties of the polymer electrolytes were further explored. It was concluded that the carrier membrane with a phase transition time of 40 h and the prepared electrolyte had the best performance. The ionic conductivity of the sample was 1.02 × 10⁻³ S/cm at 25 °C and 3.42 × 10⁻³ S/cm at 60 °C. At its best cycle performance, it had the highest discharge-specific capacity of 155.6 mAh/g, and after 70 cycles, the discharge-specific capacity was 152.4 mAh/g, with a capacity retention rate of 98% and a discharge efficiency close to 100%. At the same time, the thermogravimetric curves showed that the samples prepared by this process had good thermal stability which can meet the various requirements of lithium-ion batteries. Full article

(This article belongs to the Special Issue Solid State Batteries: From Materials Research to Design and Applications)

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10 pages, 2299 KiB

Open AccessArticle

Epoxy Resin-Reinforced F-Assisted Na₃Zr₂Si₂PO₁₂ Solid Electrolyte for Solid-State Sodium Metal Batteries

by Yao Fu, Dangling Liu, Yongjiang Sun, Genfu Zhao and Hong Guo

Batteries 2023, 9(6), 331; https://doi.org/10.3390/batteries9060331 - 19 Jun 2023

Cited by 2 | Viewed by 1924

Abstract

Solid sodium ion batteries (SIBs) show a significant amount of potential for development as energy storage systems; therefore, there is an urgent need to explore an efficient solid electrolyte for SIBs. Na₃Zr₂Si₂PO₁₂ (NZSP) is regarded as one of the most potential solid-state electrolytes (SSE) for SIBs, with good thermal stability and mechanical properties. However, NZSP has low room temperature ionic conductivity and large interfacial impedance. F⁻doped NZSP has a larger grain size and density, which is beneficial for acquiring higher ionic conductivity, and the composite system prepared with epoxy can further improve density and inhibit Na dendrite growth. The composite system exhibits an outstanding Na⁺ conductivity of 0.67 mS cm⁻¹ at room temperature and an ionic mobility number of 0.79. It also has a wider electrochemical stability window and cycling stability. Full article

(This article belongs to the Special Issue Solid State Batteries: From Materials Research to Design and Applications)

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11 pages, 2721 KiB

Open AccessArticle

Engineered Grain Boundary Enables the Room Temperature Solid-State Sodium Metal Batteries

by Yang Li, Zheng Sun, Haibo Jin and Yongjie Zhao

Batteries 2023, 9(5), 252; https://doi.org/10.3390/batteries9050252 - 27 Apr 2023

Cited by 11 | Viewed by 2143

Abstract

The NASICON-type (Sodium Super Ionic Conductor) Na₃Zr₂Si₂PO₁₂ solid electrolyte is one of the most promising electrolytes for solid-state sodium metal batteries. When preparing Na₃Zr₂Si₂PO₁₂ ceramic using a traditional high-temperature solid-state reaction, the high-densification temperature would result in the volatilization of certain elements and the consequent generation of impurity phase, worsening the functional and mechanical performance of the NASICON electrolyte. We rationally introduced the sintering additive B₂O₃ to the NASICON matrix and systemically investigated the influence of B₂O₃ on the crystal structure, microstructure, electrical performance, and electrochemical performance of the NASICON electrolytes. The results reveal that B₂O₃ can effectively reduce the densification sintering temperature and promote the performance of the Na₃Zr₂Si₂PO₁₂ electrolyte. The Na₃Zr₂Si₂PO₁₂-2%B₂O₃-1150 ℃ achieves the highest ionic conductivity of 4.7 × 10⁻⁴ S cm⁻¹ (at 25 °C) with an activation energy of 0.33 eV. Furthermore, the grain boundary phase formed during the sintering process could improve the mechanical behavior of the grain boundary and inhibit the propagation of metallic sodium dendrite within the NASICON electrolyte. The assembled Na/Na₃Zr₂Si₂PO₁₂-2%B₂O₃/Na₃V_1.5Cr_0.5(PO₄)₃ cell reveals the initial discharge capacity of 98.5 mAh g⁻¹ with an initial Coulombic efficiency of 84.14% and shows a capacity retention of 70.3% at 30 mA g⁻¹ over 200 cycles. Full article

(This article belongs to the Special Issue Solid State Batteries: From Materials Research to Design and Applications)

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14 pages, 13179 KiB

Open AccessArticle

Grain Boundary Characterization and Potential Percolation of the Solid Electrolyte LLZO

by Shuo Fu, Yulia Arinicheva, Claas Hüter, Martin Finsterbusch and Robert Spatschek

Batteries 2023, 9(4), 222; https://doi.org/10.3390/batteries9040222 - 8 Apr 2023

Cited by 8 | Viewed by 2644

Abstract

The influence of different processing routes and grain size distributions on the character of the grain boundaries in Li

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(LLZO) and the potential influence on failure through formation of percolating lithium metal networks in the solid [...] Read more.

The influence of different processing routes and grain size distributions on the character of the grain boundaries in Li

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(LLZO) and the potential influence on failure through formation of percolating lithium metal networks in the solid electrolyte are investigated. Therefore, high quality hot-pressed Li

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pellets are synthesised with two different grain size distributions. Based on the electron backscatter diffraction measurements, the grain boundary network including the grain boundary distribution and its connectivity via triple junctions are analysed concerning potential Li plating along certain susceptible grain boundary clusters in the hot-pressed LLZO pellets. Additionally, the study investigates the possibility to interpret short-circuiting caused by Li metal plating or penetration in all-solid-state batteries through percolation mechanisms in the solid electrolyte microstructure, in analogy to grain boundary failure processes in metallic systems. Full article

(This article belongs to the Special Issue Solid State Batteries: From Materials Research to Design and Applications)

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11 pages, 2877 KiB

Open AccessEditor’s ChoiceArticle

In Situ Solidified Gel Polymer Electrolytes for Stable Solid−State Lithium Batteries at High Temperatures

by Junfeng Ma, Zhiyan Wang, Jinghua Wu, Zhi Gu, Xing Xin and Xiayin Yao

Batteries 2023, 9(1), 28; https://doi.org/10.3390/batteries9010028 - 30 Dec 2022

Cited by 11 | Viewed by 4895

Abstract

Lithium metal batteries have attracted much attention due to their high energy density. However, the critical safety issues and chemical instability of conventional liquid electrolytes in lithium metal batteries significantly limit their practical application. Herein, we propose polyethylene (PE)−based gel polymer electrolytes by in situ polymerization, which comprise a PE skeleton, polyethylene glycol and lithium bis(trifluoromethylsulfonyl)imide as well as liquid carbonate electrolytes. The obtained PE−based gel polymer electrolyte exhibits good interfacial compatibility with electrodes, high ion conductivity, and wide electrochemical window at high temperatures. Moreover, the assembled LiFePO₄//Li solid−state batteries employing PE−based gel polymer electrolyte with 50% liquid carbonate electrolytes deliver good rate performance and excellent cyclic life at both 60 °C and 80 °C. In particular, they achieve high specific capacities of 158.5 mA h g⁻¹ with a retention of 98.87% after 100 cycles under 80 °C at 0.5 C. The in situ solidified method for preparing PE−based gel polymer electrolytes proposes a feasible approach for the practical application of lithium metal batteries. Full article

(This article belongs to the Special Issue Solid State Batteries: From Materials Research to Design and Applications)

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Review

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19 pages, 3951 KiB

Open AccessReview

Progress on Designing Artificial Solid Electrolyte Interphases for Dendrite-Free Sodium Metal Anodes

by Pengcheng Shi, Xu Wang, Xiaolong Cheng and Yu Jiang

Batteries 2023, 9(7), 345; https://doi.org/10.3390/batteries9070345 - 27 Jun 2023

Cited by 9 | Viewed by 2603

Abstract

Nature-abundant sodium metal is regarded as ideal anode material for advanced batteries due to its high specific capacity of 1166 mAh g⁻¹ and low redox potential of −2.71 V. However, the uncontrollable dendritic Na formation and low coulombic efficiency remain major obstacles to its application. Notably, the unstable and inhomogeneous solid electrolyte interphase (SEI) is recognized to be the root cause. As the SEI layer plays a critical role in regulating uniform Na deposition and improving cycling stability, SEI modification, especially artificial SEI modification, has been extensively investigated recently. In this regard, we discuss the advances in artificial interface engineering from the aspects of inorganic, organic and hybrid inorganic/organic protective layers. We also highlight key prospects for further investigations. Full article

(This article belongs to the Special Issue Solid State Batteries: From Materials Research to Design and Applications)

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21 pages, 3995 KiB

Open AccessReview

Recent Advances in Ionic Liquids—MOF Hybrid Electrolytes for Solid-State Electrolyte of Lithium Battery

by Ruifan Lin, Yingmin Jin, Yumeng Li, Xuebai Zhang and Yueping Xiong

Batteries 2023, 9(6), 314; https://doi.org/10.3390/batteries9060314 - 6 Jun 2023

Cited by 4 | Viewed by 3758

Abstract

Li-ion batteries are currently considered promising energy storage devices for the future. However, the use of liquid electrolytes poses certain challenges, including lithium dendrite penetration and flammable liquid leakage. Encouragingly, solid electrolytes endowed with high stability and safety appear to be a potential solution to these problems. Among them, ionic liquids (ILs) packed in metal organic frameworks (MOFs), known as ILs@MOFs, have emerged as a hybrid solid-state material that possesses high conductivity, low flammability, and strong mechanical stability. ILs@MOFs plays a crucial role in forming a continuous interfacial conduction network, as well as providing internal ion conduction pathways through the ionic liquid. Hence, ILs@MOFs can not only act as a suitable ionic conduct main body, but also be used as an active filler in composite polymer electrolytes (CPEs) to meet the demand for higher conductivity and lower cost. This review focuses on the characteristic properties and the ion transport mechanism behind ILs@MOFs, highlighting the main problems of its applications. Moreover, this review presents an introduction of the advantages and applications of Ils@MOFs as fillers and the improvement directions are also discussed. In the conclusion, the challenges and suggestions for the future improvement of ILs@MOFs hybrid electrolytes are also prospected. Overall, this review demonstrates the application potential of ILs@MOFs as a hybrid electrolyte material in energy storage systems. Full article

(This article belongs to the Special Issue Solid State Batteries: From Materials Research to Design and Applications)

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45 pages, 5700 KiB

Open AccessReview

Recent Progress and Perspectives of Solid State Na-CO₂ Batteries

by Zelin Wang, Chunwen Sun, Liang Lu and Lifang Jiao

Batteries 2023, 9(1), 36; https://doi.org/10.3390/batteries9010036 - 4 Jan 2023

Cited by 6 | Viewed by 3749

Abstract

Solid state Na-CO₂ batteries are a kind of promising energy storage system, which can use excess CO₂ for electrochemical energy storage. They not only have high theoretical energy densities, but also feature a high safety level of solid-state batteries and low cost owing to abundant sodium metal resources. Although many efforts have been made, the practical application of Na-CO₂ battery technology is still hampered by some crucial challenges, including short cycle life, high charging potential, poor rate performance and lower specific full discharge capacity. This paper systematically reviews the recent research advances in Na-CO₂ batteries in terms of understanding the mechanism of CO₂ reduction, carbonate formation and decomposition reaction, design strategies of cathode electrocatalysts, solid electrolytes and their interface design. In addition, the application of advanced in situ characterization techniques and theoretical calculation of metal–CO₂ batteries are briefly introduced, and the combination of theory and experiment in the research of battery materials is discussed as well. Finally, the opportunities and key challenges of solid-state Na-CO₂ electrochemical systems in the carbon-neutral era are presented. Full article

(This article belongs to the Special Issue Solid State Batteries: From Materials Research to Design and Applications)

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