JOURNAL OF MATERIALS SCIENCE
·
2024
·Vol. 59
·期 7
·3009-3017
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IF 3.5
Fu Yuan,Gong Zhemin,Li Dapeng,Liu Yongxing,Zhou Xiaolong,Yang Yong,Jiao Qing
Solid electrolytes equipped battery show promise in solving energy storage and ecological concerns owing to their excellent electrical conductivity and chemical stability. Only a limited number of substances satisfy the demanding criterion of high ionic conductivity (≥ 10 −3 S/cm), while using non-toxic elements. In this work, the designed Na 3.3 Zn 0.1 Sb 0.9 S 4 electrolyte, a zinc-doped sodium sulfide ion conductor, with a maximum conductivity of 1.48 × 10 −3 S/cm under normal conditions, and a low activation energy of 0.128 eV was achieved. This was ruled by substituting low-valence Zinc for antimony in the SbS 4 3− cell, maintaining efficient ion transport pathways. Additionally, the electrolyte demonstrated strong air stability under humid conditions and emitted minimal H 2 S. The origin of heterovalent ion doping and the impact of thermal effects on electrochemical performance were discussed in detail, which were crucial to promote the development of sodium-ion solid electrolytes.
研究领域:
材料科学
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电化学
·
能源存储
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 31
·2203095
·
IF 19.924
Lin Li,Ruonan Xu,Long Zhang,Ziqi Zhang,Meng Yang,Di Liu,Xinlin Yan,Aijun Zhou
The severe parasitic interface reaction and dendrite growth retard the practical applications of all-solid-state (ASS) Na batteries with sulfide solid electrolytes (SEs). Here, a novel composite SE is proposed, with a high ionic conductivity, composed of Na 3 SbS 4 (NSS) and oxysulfide glass. The study reveals that the P 2 S 7- a O a and PS 4- a O a units in oxysulfide play various roles: The former is deoxidized to release free O ions, which reacts with the anode via migrating to form oxides, favoring an improved interface stability. The latter is highly stable upon cycling, thereby maintaining an ion transport network. Meanwhile, NSS acts as a dendrite predator via reacting with penetrated Na. These advantages enable the resulting ASS Na battery with superior long-term cycling performance at a high current density at room temperature, one of the best results so far. This discovery sheds light on innovative advanced SE materials through an oxysulfide-based composite design.
研究领域:
材料科学
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电化学
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电池技术
✓ 已验证
DOI
高影响因子
Batteries & Supercaps
·
2022
·Vol. 6
·期 1
·e202200353
·
IF 6.043
Yayu Guo,Xixi Shi,Yue Ma,Dawei Song,Hongzhou Zhang,Chunliang Li,Lianqi Zhang
Antimony-based sulfide solid electrolyte Na 3 SbS 4 with good moisture stability is attractive for practical application in all-solid-state sodium batteries. Liquid-phase reaction is a facile and widely-used strategy, but the specific reactions in synthetic process and related mechanisms are still unclear. Herein, the reaction processes of synthesizing Na 3 SbS 4 by liquid-phase reaction of Na 2 S, Sb 2 S 3 and S in acetonitrile (ACN) are extensively investigated. A colorless supernatant and dark green precipitate are obtained after reacting for 24 h, the raw materials are negligible in supernatant. More importantly, the post-treatment temperature is investigated and the tetragonal Na 3 SbS 4 (t-Na 3 SbS 4 ) with high ionic conductivity (0.46 mS cm −1 at 25 °C) is obtained after heating at 450 °C for 3 h. Remarkably, the direct stacking of electrolyte is developed and t-Na 3 SbS 4 is further prepared into a free-standing sheet-type solid electrolyte membrane using polytetrafluoroethylene (PTFE) fibrillation, then an ionic conductivity is achieved (0.17 mS cm −1 at 25 °C). Graphical Solid electrolyte ! The reaction processes of synthesizing Na 3 SbS 4 by liquid-phase reaction using acetonitrile are extensively investigated, and tetragonal Na 3 SbS 4 with high ionic conductivity (0.46 mS cm −1 ) is obtained after heating at 450 °C. Remarkably, the tetragonal Na 3 SbS 4 is further prepared into a sheet-type electrolyte membrane (0.17 mS cm −1 ) using polytetrafluoroethylene.
研究领域:
材料科学
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电化学
·
储能
·
固态化学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry C
·
2023
·Vol. 11
·期 45
·15967-15978
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IF 6.4
Zhemin Gong,Lingjun Shu,Jingxuan Yin,Chengwei Gao,Yongxing Liu,Xiaolong Zhou,Xiang Shen,Shixun Dai,Changgui Lin,Qing Jiao
Solid electrolytes are promising candidates for addressing energy and environmental problems due to their excellent electrical conductivity and extremely high safety. To date, only a few alternative materials can meet the high ionic conductivity requirements of at least ≥1 mS cm−1 when using nontoxic and economical elements. For the first time, we report an Mn-doped sodium sulfide ion conductor Na3.24Mn0.08Sb0.92S4 that shows a maximum conductivity of 2.05 × 10−3 S cm−1 at 25 °C. In its sulfide superionic conductor structure, the antimony in the SbS43− cell is replaced with manganese with a low valence state, maintaining a good transport pathway and accelerating ion transport. This electrolyte exhibits good air stability in a humid environment and minimal H2S release. Moreover, its ionic conductivity is almost unchanged after the conductor is stored at room temperature for many days, which is crucial for promoting the development of sodium ion solid electrolytes. The stability of the conductor and sodium metal has also been evaluated, further studying its potential for practical applications.
研究领域:
材料科学
·
能源存储与转换
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Zhemin Gong,Lingjun Shu,Jingxuan Yin,Chengwei Gao,Yongxing Liu,Xiaolong Zhou,Xiang Shen,Shixun Dai,Changgui Lin,Qing Jiao
Here, we report the SiS 2 –NaBr double-doped sulfide superionic conductor Na 3.02 Si 0.1 Sb 0.9 S 3.92 Br 0.08 . The dual-doping effect of SiS 2 and NaBr in the Na 3 SbS 4 electrolyte was investigated by mechanical ball milling and high-temperature heat treatment. The improved glass–ceramic Na 3.02 Si 0.1 Sb 0.9 S 3.92 Br 0.08 solid electrolyte obtained a high ionic conductivity of 2.26 × 10 −3 S/cm and a low activation energy of 0.077 eV (0.25 eV for Na 3 SbS 4 ) at room temperature. Moreover, the electrochemical property test was characterized by a higher critical current density of 1.228 mA/cm 2 (0.585 mA/cm 2 for Na 3 SbS 4 ) and stable cycling at 0.1 mA cm −2 current densities exceeding 120 h (50.33 h for Na 3 SbS 4 ). Some Si atoms occupying the Sb position greatly contributed to the formation of the Na 3 SbS 4 high-ionic conductive phase. The introduction of an appropriate amount of halogen improved the compactness of the sample and nearly suppressed the majority of H 2 S release from the original electrolyte. The substitution effect and the ion conduction structure were analyzed in detail.
研究领域:
材料科学
·
电化学
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能源存储
✓ 已验证
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2020
·
IF 6.155
Haonan Cao,Meiqi Yu,Long Zhang,Zhaoxing Zhang,Xinlin Yan,Peng Li,Chuang Yu
Solution-synthesis method is attractive for solid electrolytes because it is a facile and scalable process to be used to permeate electrodes and to construct a thin electrolyte coating layer on active materials. In this work, we report Cl-doped Na 3 SbS 4 prepared via aqueous-solution approach. Besides decent ionic conductivity , the aqueous-solution approached electrolyte demonstrates an improved interfacial stability toward Na metal compared to the solid-state sintered one because of the residual hydrate, nanosized microstructure, and Cl incorporation. All-solid-state batteries using the solution-prepared electrolytes have enhanced cycling performance, though the performance still needs to be further improved.
研究领域:
材料科学
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电化学
·
储能
·
固态电池
✓ 已验证
DOI
高影响因子
Nano Energy
·
2019
·
IF 15.548
Hongli Wan,Jean Pierre Mwizerwa,Fudong Han,Wei Weng,Jing Yang,Chunsheng Wang,Xiayin Yao
A nanoscaled Na 3 SbS 3.75 Se 0.25 solid electrolyte with less grain-boundary resistance was synthesized using a liquid/solid fusion technology. The Na 3 SbS 3.75 Se 0.25 solid electrolyte shows a high ionic conductivity of 4.03 × 10 −3 S cm −1 at room temperature due to the significantly decreased amorphous phase in the electrolyte. Moreover, the small particle size of the solid electrolytes enhances the contact between solid electrolyte and electrode, reducing the interfacial contact resistance. As a result, FeS 2 /Na 3 SbS 3.75 Se 0.25 /Na all-solid-state sodium batteries achieve a high specific capacity of 140.6 mAh g −1 for 300 cycles at a high current of 500 mA g −1 . In addition, FeS 2 /Na 3 SbS 3.75 Se 0.25 /Na cells also demonstrate a high rate-capacity of 365.3, 301.8, 210.1 and 96.0 mAh g −1 at current densities of 50, 300, 500 and 1000 mA g −1 , respectively. The liquid/solid fusion technology is a unique synthesis strategy to develop superionic electrolytes for room temperature all-solid-state sodium secondary battery.
研究领域:
材料科学
·
电化学
·
储能
·
固态离子学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zhiwen Wang,Long Zhang,Xiong Shang,Weizhe Wang,Xinlin Yan,Chuang Yu,Li-min Wang
Na 3 SbS 4 -based solid electrolytes show the merits of a high ionic conductivity and aqueous-processible syntheses. However, Na 3 SbS 4 (NSS) is incompatible with metallic Na and Na alloys. Incorporation of an ionic liquid can solve this issue, but it is hard to coat it on sulfide powders homogeneously in a minimal quantity. Herein, a facile preparation is realized by using a PVDF filtration membrane with submicro-size vertical channels to constrain the flow of the liquid. By this constraint effect, the well mixed BMPTFSI and a NSS aqueous solution are soaked by the vertical channels and inhibited the segregation. Homogeneous BMPTFSI coating layers on NSS particles with a thickness less than 500 nm are encapsulated in the vertical channels after evaporating the water. The coating layers not only improve the physical contact of the NSS particles for enhanced ion transport, but more importantly effectively stabilize the interface between NSS and the metallic Na. The Na 3 V 2 (PO 4 ) 3 ||Na half cells with this composite electrolyte demonstrate superior cycling stability and good rate capability. This green method provides a facile way to optimize the interfacial performance for solid state batteries using ionic liquid.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
Nano Energy
·
2026
·
IF 17.1
Yi Tang,Shoumeng Yang,Congcong Liu,Yu Yao,Zhijun Wu,Wubin Du,Hongge Pan,Yang Yang,Xianhong Rui,Yan Yu
All-solid-state Na-S batteries (ASSNSBs) are promising candidates for grid-scale energy storage owing to their high energy density and intrinsic safety. However, the practical utilization of Na 3 SbS 4 (NSS) as a solid electrolyte is hindered by its limited intrinsic Na + transport capability. Drawing on insights from first-principles analysis of aliovalent doping and vacancy formation, we design and synthesize Ca-doped NSS electrolytes with enhanced ionic conductivity and improved compatibility with Na 3 Sn alloy anodes. The optimized Na 2.9 Ca 0.05 SbS 4 (NCSS-0.05) achieves a room-temperature ionic conductivity of 0.51 mS cm −1 and a reduced activation energy of 0.237 eV, alongside highly stable symmetric cell cycling for over 400 h. When incorporated into ASSNSBs, NCSS-0.05 enables an initial discharge capacity of 1601 mAh g −1 at 0.17 A g −1 and maintains 97.2 % capacity retention over 250 cycles at 0.5 A g −1 . Moreover, the Ca-modified electrolyte exhibits strong compatibility with various sulfide-based cathodes, including TiS 2 and VS 2 , further demonstrating its broad applicability. These results establish a robust aliovalent-doping strategy for engineering fast-ion-conducting sulfide solid electrolytes and advancing high-performance all-solid-state sodium battery technologies.
✓ 已验证
产品关联
DOI
高影响因子
Applied Materials Today
·
2022
·
IF 8.663
Wei Weng,Gaozhan Liu,Yunming Li,Lin Shen,Xiayin Yao
Development of sodium solid electrolytes with high ionic conductivity and good interface stability towards Na metal plays a dominant role in achieving stable all-solid-state sodium batteries. Herein, WS 2 -doped Na 3- x Sb 1- x W x S 4 and WO 2 -doped Na 3- x Sb 1- x W x S 4–2 x O 2 x ( x = 0.025, 0.05, 0.075, 0.1) solid electrolytes are successfully synthesized by melt-quenching method followed by an annealing procedure. Compared with 0.98 mS cm −1 for pristine Na 3 SbS 4 , the dramatically enhanced room temperature ionic conductivities of 10.37 and 8.49 mS cm −1 are achieved for Na 2.95 Sb 0.95 W 0.05 S 4 and Na 2.95 Sb 0.95 W 0.05 S 3.9 O 0.1 , respectively. In addition, it is found that the introduction of oxygen in Na 3 SbS 4 through W and O co-doping can alleviate the deteriorative Na/solid electrolyte interface induced by W substitution. The modified interface stability is demonstrated by the suppressed increase of Na plating/striping voltage and impedance for the symmetric Na/Na 2.95 Sb 0.95 W 0.05 S 3.9 O 0.1 /Na cells. Moreover, in contrast with rapid capacity decay for TiS 2 /Na 2.95 Sb 0.95 W 0.05 S 4 /Na battery, the batteries employing Na 2.95 Sb 0.95 W 0.05 S 3.9 O 0.1 exhibit stable cyclic performance and good rate capability. This work provides a W and O co-doping strategy for preparing Na 3 SbS 4 solid electrolytes with simultaneously enhanced ionic conductivity and interface stability.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Energy Materials
·
2026
·Vol. 6
·期 6
·N
·
IF 11.9
Celastin Bebina Thairiyarayar,Fu-Ming Wang,Soorathep Kheawhom,Jeng-Kuei Chang,Wei-Ren Liu
All-solid-state batteries are regarded as promising next-generation energy-storage systems due to their potential to achieve energy densities exceeding 400 Wh kg-1. However, their practical implementation remains limited by interfacial instability, non-uniform metal deposition, and continuous electrolyte decomposition during cycling. In this work, a dual-sided polymer coating was introduced onto Na3SbS4 solid electrolyte pellets using a siloxane-based sodiated polyelectrolyte (AAM950), combined with sodium bis(trifluoromethylsulfonyl)imide, as an artificial interfacial layer. The conformal coating partially filled surface pores and reduced interfacial gaps, leading to improved solid-solid contact between the electrolyte and electrode. The optimized 7 µL polymer-coated Na3SbS4 (NSS) pellet exhibited an ionic conductivity of 0.348 mS cm-1 at 55 °C. In addition, the Na2/3Fe1/2Mn1/2O2|Na-AAM950-NSS-Na-AAM950|Na cell delivered an initial discharge capacity of 137.4 mAh g-1, compared with 83.59 mAh g-1 for the bare NSS system at 0.02 A g-1, together with a capacity retention of 89.6% and an average Coulombic efficiency of 99.56% over 50 cycles at 55 °C. Although the polymer layer did not substantially increase the intrinsic bulk ionic conductivity of NSS, it effectively stabilized the electrode/electrolyte interface and promoted more homogeneous Na+ transport during cycling. These findings demonstrate that dual-sided polymer modification provides an effective strategy for improving the practical cycling stability of Na3SbS4-based sodium all-solid-state batteries.
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry C
·
2024
·Vol. 12
·期 47
·19296-19306
·
IF 5.7
Tao Huan,Jingxuan Yin,Yu Shen,Jingxin Lu,Chengwei Gao,Yongxing Liu,Shixun Dai,Changgui Lin,Xianghua Zhang,Hongli Ma,Xiang Shen,Qing Jiao
All-solid-state sodium-ion batteries are emerging as a highly promising substitute for lithium-ion batteries, primarily owing to their rich natural resources and superior safety performance. Solid electrolytes are integral components of all-solid-state batteries and have attracted much attention due to their remarkable safety and chemical stability. This study examines a novel solid electrolyte Na3(WSn)xSb1−2xS4 by modifying the W/Sn ratio and achieves a high ionic conductivity of 11.3 mS cm−2 at room temperature. Structural analysis demonstrates that the inclusion of tungsten facilitates the formation of cubic phase Na3SbS4 by more sodium vacancies. Furthermore, the co-dopant Sn ensures pure cubic conductors by removing impurities WS2 and increasing the element solubility. This efficiently enhances the movement of sodium ions and promotes ion transportation. The W/Sn-optimized Na3SbS4 (NBS) electrolyte also exhibited stable cycling for about 323 hours, which is about eight times longer than the Na3SbS4 base electrolyte. The efficient enhancement of the critical current density demonstrated the improvement of the structural stability at the interface where sodium dendrites formed easily. The formed Na–Sn alloy provides a protective barrier for the normal transport of ions. In addition, the small release of H2S also proves the stability of the electrolyte structure. These characteristics make it a highly promising electrolyte material for all-solid-state electrolytes.
研究领域:
材料科学
·
电化学
·
储能技术
·
固态离子学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）