Energy Material Advances
·
2025
·
IF 15.9
Mengqi Wu,Shengyao Luo,Tonghui Xu,Tianle Zheng,Zhengzheng Ru,Said Amzil,Yiyao Xiao,Yinghui Li,Meilan Peng,Wenwen Xue,Jie Gao,Yunfang Gao,Ya-Jun Cheng,Peter Müller-Buschbaum,Yonggao Xia
Lithium metal batteries (LMBs) have attracted much attention due to their high specific capacity. However, commercial carbonate electrolytes are challenging to apply in LMBs because of the narrow operating temperature range (−20 to 50 °C). Carboxylate solvents have the advantages of low viscosity and low freezing point and perform well at low temperatures. However, their poor thermal stability limits their application at high temperatures. This work added a dinitrile solvent to the carboxylate electrolyte to expand its liquid range and improve its electrochemical stability. In addition, the coordination of molecules in the first solvated layer is carefully controlled to promote many anions entering the solvated layer, contributing to forming a robust inorganic solid electrolyte interface film. Because of the addition of the dinitrile solvent, the electrolyte enables Li/NCM811 cells to achieve a capacity release of 149.3 mAh/g at −40 °C. After 200 cycles at 80 °C, the capacity retention rate of Li/LFP cells is 94.31%. Even in ultra-thin lithium metal cells (17 μm), it can be stable for more than 100 cycles. This opens up new opportunities for developing electrolytes suitable for high-performance and all-weather LMBs.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
Energy Storage Materials
·
2024
·
IF 18.9
Shiyao Chen,Qingkui Peng,Zesen Wei,Yuxuan Li,Yongbing Yue,Yue Zhang,Wei Zeng,Kaiqiang Jin,Lihua Jiang,Qingsong Wang
Replacing flammable non-aqueous organic liquid electrolyte (LE) with high thermal stability solid-state electrolyte (SSE) is considered to overcome the safety issues in lithium metal batteries (LMBs). However, both inorganic solid-state batteries (SSBs) with high mechanical strength and thermal stability, as well as flexible polymer-based SSBs, are not proven to be inherently safe yet. Currently, the reliability of SSBs still require continuous scientific verification. In this work, quasi-solid-state electrolyte (QSE) with practical application prospects was prepared through in-situ polymerization method. The effects of QSE and LE on the thermal runaway behavior of LMBs were systematically compared from four levels: electrolyte, electrolyte/electrode interface, coin cells, and pouch cells. The results showed that higher thermal stability of QSE was conducive for improving the reliability of quasi-solid-state batteries (QSBs) under different abused conditions. The stable and dense solid electrolyte interface (SEI) in QSB could not only inhibit the severe side-reactions of LMBs during cycling at elevated temperature, but also enhance the decomposition temperature with dead lithium. QSE's lower reaction activity towards Li reduced the exothermic reaction inside the battery had been proven to increase the self-exothermic onset temperature and thermal runaway trigger temperature of LMBs, which promoted the safety performance of LMBs. Thus, this study revealed the thermal runaway mechanism of QSE in LMBs, and provided a theoretical guideline for safe QSBs design.
研究领域:
材料科学
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能源技术
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
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IF 19
Zhaowei Sun,Ronghou Yao,Yingshan Huang,Jin Wu,Caiju Li,Jianhong Yi,Shizhao Xiong,Hongying Hou,Hengxing Ji
Sodium (Na) metal anode is the essential component of low-cost and high-performance Na metal batteries, yet its application is hampered by the unstable anode/electrolyte interface and inevitable growth of Na dendrites. In this work, a hierarchically porous artificial surface layer with sodiophilic silver (Ag) nanoparticles decorating the bottom surface (HPFA) is reported, which can regulate the uniform deposition of Na and eliminate the local overgrowth of dendrites on the surface of Na substrate. The dependence of Na deposition behavior on the hierarchical structure of surface layers is revealed by operando optical microscopy and multiphysics simulation, indicating the multifunction of the HPFA layer in stabilizing the Na anode during the electrochemical plating/stripping process. The as-fabricated HPFA/Na anode depicts prolonged life-span and improved stability in both ether and carbonate electrolytes, while the symmetric cell shows no sign of short-circuit even after 1200 h of repeated charging/discharging at 2 mA cm −2 with a high area capacity of 4 mAh cm −2 . Besides, when the HPFA/Na anode is paired with Na 3 V 2 (PO 4 ) 3 cathode and ether electrolyte, the full cell exhibits a low decay rate of ≈0.28% with a stable coulombic Efficiency value of ≈99.88% at 2 C rate.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
产品关联
DOI
高影响因子
Energy Storage Materials
·
2022
·
IF 20.831
Long Chen,Jianhao Lu,Yibo Wang,Pan He,Shaobo Huang,Yan Liu,Yanzhou Wu,Gaoping Cao,Li Wang,Xiangming He,Jingyi Qiu,Hao Zhang
Lithium ion batteries (LIBs) have swept the whole energy storage field. However, the current mainstream lithium batteries are difficult to operate stably at high temperature (>60°C) due to the decomposition of electrolyte and solid electrolyte interphase (SEI), the cathode metal elements dissolution behavior, and potential thermal runaway. Here, We report a double-salt electrolyte with lithium bis(fluorosulfonyl)imide (LiFSI) and lithium difluoro(oxalato)borate (LiDFOB) as electrolyte salt, fluoroethylene carbonate (FEC), and tetra(ethylene glycol) dimethyl ether (TEGDME) as cosolvent, which delivers excellent ionic conductivity, high electrochemical stability and satisfactory ability to impede the dissolution of Fe element under elevated temperature (70°C). In addition, the electrolyte is benefited to form a robust and thermal-resistance solid-electrolyte interface (SEI) layer on the surface of graphite (Gr) anode, which shows improved decomposition temperature (86°C). The assembled thermally stable and high-safety 1300 mAh 18650-type LiFePO 4 |Gr cell shows high Coulombic efficiency (∼99.7%), improved cycling stability with discharge capacity 871.1 mAh after 200 cycles at 0.5 C and 70°C. This work affords a splendid strategy for address the unstable interface at both cathode and anode for safe high-temperature LIBs.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Meng Wei,Pengfei Zhai,Yihan Li,Xin Zhao,Jiancheng Li,Tao Zhang,Guanghui Liu,Zhanjun Yu,Song Xu
The NASICON-type ceramic Li 1·5 Al 0.5 Ge 1.5 (PO4) 3 (LAGP) electrolyte has been proposed as the most competitive candidates of electrolyte materials toward solid-state Li metal batteries (LMBs) by reason of its high ionic conductivity , cyclic stability under extreme temperatures and wide voltage window. However, poor interface contact, high interfacial resistance and intractable mechanical properties greatly limit its practical applications. In this work, an inorganic-polymer “LAGP in PVDF” quasi-solid-state electrolyte (QSSE) is developed via solution casting method, in which pyr14TFSI ionic liquid (IL) and LiTFSI are combined as functional wetting interface . Benefiting from the coherent interaction of LAGP nanoparticles incorporated into the polymer matrix , and inherent protection of IL, the overall performance of the optimized QSSE include thermal stability, dense structure, flexibility and electrochemical properties . The XRD, SEM, XPS tests demonstrate that the IL using as a solid/electrolyte modified interlayer can enhance Li + transport, interfacial infiltration and homogenize lithium deposition. The LiFePO 4 |PL-25LAGP|Li solid-state battery presents an excellent circulation performance under ambient temperature, which displayed an initial discharge specific capacity of 146.8 mAh g −1 at 0.5C and capacity retention of 96.25 % after 150 cycles. The flexibility PL-LAGP CSE shows superior safety and greater development potential for the “LAGP in PVDF” composite electrolyte in solid state LMBs.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Chunpeng Li,Jun Zhang,Kai Zhang,Anping Zhang,Wei Jian,Ping Jiang,Zhong-Shuai Wu,Dianbo Ruan
Aqueous Na–Zn ion batteries are promising for large-scale energy storage due to their low cost and high output voltage potential. However, the formed dendrites and notorious side reactions of zinc anodes lead to rapid performance degradation. Here, a sodium–zinc dication hybrid hydrated deep eutectic electrolyte system (NZDES) is proposed, in which organic ligands and all water molecules participate in NZDES’s internal solvation structure networks, resulting in the suppressed side reaction at the Zn anode. Furthermore, the unique aqueous Zn2+ solvation shell is efficiently regulated by Na+, enabling high Zn deposition/stripping reversibility (96.5% Coulombic efficiency). Meanwhile, the decomposition of solvated methylsulfonylmethane (MSM) forms the enhanced solid electrolyte interphase, which improves the smoothness of the Zn anode and further suppresses the decomposition of water. With these merits, the CuHCF/Zn hybrid batteries with dication deep eutectic electrolytes exhibit a high capacity retention of >91.6% after 3000 cycles at 10 C with a 1.9 V open circuit voltage. The results provide a potential design strategy for an effective solid electrolyte interface for aqueous zinc ion batteries.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
Sustainable Energy & Fuels
·
2022
·Vol. 6
·期 5
·1281-1288
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IF 6.813
Xiaofei Wang,Wenjun He,Haoliang Xue,Daoming Zhang,Jin Wang,Lina Wang,Jun Li
Lithium (Li) metal batteries (LMBs) have been considered as promising candidates for next-generation energy storage devices due to the tremendous advantages of Li-metal anodes. However, poor cycling stability and severe safety issues impede the practical application of LMBs. Herein, a nonflammable phosphate-based localized high-concentration electrolyte composed of lithium difluoro(oxalato)borate/dimethyl methyl phosphonate/1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropylether (LiDFOB–DMMP/HFE) is proposed to improve the safety and reversibility of high-voltage LMBs simultaneously. Replacing highly flammable conventional solvents in the electrolyte with flame-retardant DMMP greatly reduces the fire risks of the electrolyte. The dominant reduction of DFOB− anions induces a robust and LiF-rich solid-electrolyte interphase on the Li-metal anode, stabilizing the Li metal/electrolyte interface and leading to dendrite-free Li deposition. An effective cathode electrolyte interphase is generated as well to inhibit structural degradation and transition-metal dissolution of the high-voltage LiNi6Mn2Co2O2 (NMC622) cathode. Moreover, the electrolyte displays a high oxidative stability potential of >5.0 V. Thus, the Li‖NMC622 battery using LiDFOB–DMMP/HFE electrolyte exhibits a superior cyclability with no capacity loss and a high average coulombic efficiency of 99.6% over 100 cycles under a high cutoff voltage of 4.5 V. This emerging electrolyte offers great potential to realize the stable cycling of high-voltage LMBs with fine safety for future applications.
研究领域:
材料科学
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电化学
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能源存储技术
✓ 已验证
DOI
高影响因子
Small
·
2024
·Vol. 20
·期 40
·2401204
·
IF 13
Siyu Fang,Chengyu Han,Shaojie Zhang,Yu Cao,Kang Ma,Yiming Zhang,Xinpeng Han,Juan Wang,Jie Sun
The demand for state-of-the-art high-energy-density lithium-ion batteries is increasing. However, the low specific capacity of electrode materials in conventional full-cell systems cannot meet the requirements. Ni-rich layered oxide cathodes such as Li(Ni 0.8 Co 0.1 Mn 0.1 )O 2 (NCM811) have a high theoretical specific capacity of 200 mAh g −1 , but it is always accompanied by side reactions on the electrode/electrolyte interface. Phosphorus anode possesses a high theoretical specific capacity of 2596 mAh g −1 , but it has a huge volume expansion (≈300%). Herein, a highly compatible and secure electrolyte is reported via introducing an additive with a narrow electrochemical window, Lithium difluoro(oxalato)borate (LiDFOB), into 1 m LiPF 6 EC/DMC with tris (2,2,2-trifluoroethyl) phosphate (TFEP) as a cosolvent. LiDFOB participates in the formation of organic/inorganic hybrid electrode/electrolyte interface layers at both the cathode and anode sides. The side reactions on the surface of the NCM811 cathode and the volume expansion of the phosphorus anode are effectively alleviated. The NCM811//RP full cell in this electrolyte shows high capacity retention of 82% after 150 cycles at a 0.5C rate. Meanwhile, the electrolyte shows non-flammability. This work highlights the importance of manipulating the electrode/electrolyte interface layers for the design of lithium-ion batteries with high energy density.
研究领域:
材料科学
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能源技术
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Hao Wu,Wanbao Wu,Lin Xie,Chaochao Gao,Erlei Zhang,Jichuan Zhang,Peng He,Jiaheng Zhang
The high reactivity of sodium leads to significant safety challenges, while the unstable solid electrolyte interphase (SEI) further complicates its use in sodium-metal batteries (SMBs), collectively impeding their path to commercialization. A deep eutectic electrolyte (DEE) is introduced, which addresses these challenges by balancing high ionic conductivity with stable SEI formation. The introduction of N-methylacetamide enhances the nonflammability of the solvent and adjusts the SEI composition. The DEE accelerates the interfacial kinetics and promotes the formation of a uniform, inorganic-rich SEI with Na2S and NaF on the sodium anode. It also extends the electrochemical stability window to 4.8 V. Additionally, the DEE exhibits high ionic conductivity, enabling fast charging of the SMBs. In a Na3V2(PO4)3||Na cell, the electrolyte achieved a capacity retention of 96% after 1,500 cycles at a current density of 5 C. These findings offer important insights for advancing the commercialization of SMBs with enhanced safety features and superior electrochemical performance.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
Joule
·
2025
·
IF 35.4
Yawei Chen,Menghao Li,Yulin Jie,Yue Liu,Zhengfeng Zhang,Peiping Yu,Wanxia Li,Yang Liu,Xinpeng Li,Zhanwu Lei,Pengfei Yan,Tao Cheng,M. Danny Gu,Shuhong Jiao,Ruiguo Cao
High-voltage lithium (Li) metal batteries (HVLMBs) have attracted tremendous research interest in the past decade owing to their high energy densities. Electrode-electrolyte interphases in HVLMBs play critical roles in dictating their electrochemical performance. However, despite the intensive research on solid-electrolyte interphase (SEI) of Li anode, the cathode-electrolyte interphase (CEI) on high-voltage cathodes remains elusive. Herein, we report the formation and dynamic evolution of CEI on LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) cathodes in ether-based electrolytes. We reveal that the solvent-derived interphase predominates the initial CEI, which subsequently evolves into a Li fluoride (LiF)-rich CEI during cycling. Through solvent design, the weak-solvation electrolyte with branched ether solvents promotes the formation of a conformal CEI layer featuring the monodispersing LiF nanocrystals (∼8 nm), thereby enabling NMC811 cathodes to sustain up to 2,000 cycles. This work addresses the long-standing questions regarding CEI evolution and provides valuable guidance for the rational electrolyte design for HVLMBs.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Storage
·
2024
·
IF 8.9
Y. Zhang,X. Lou,J. Dan,C. Franke,L. Tang,J. Li,Z. Gao,L. Zhou,B. Chen,T. Li,T. Liu
All-solid-state lithium batteries with lean (ultrathin) lithium anodes and polymer-based electrolytes e.g., polyethylene oxide (PEO), can potentially offer high energy density , reduced processing cost and improved mechanical contact at electrolyte-electrode interfaces. The non-uniform lithium deposition and inadequate mechanical strength of PEO, however, tend to cause deactivated lithium and short-circuiting by Li dendrites over lithium deposition/stripping cycles; these issues become more aggravated with lean Li anodes due to the more severe volume changes. Herein, we construct a more mechanically and chemically stable lithium-electrolyte interface by coupling alloyed lean Li anodes (<50 μm) with PEO electrolytes blended with polymers of intrinsic porosity (PIMs). The lean Li anode is fabricated by a facile and scalable cold-rolling method, which leads to a uniformly alloyed lithium anode permitting epitaxial Li deposition. Meanwhile, PIM reinforces the mechanical strength of the PEO composite electrolyte, reducing the likelihood of dendrite formation/penetration. Importantly, the introduction of both GaInSnZn and the first-generation PIM has been found to reduce the interfacial charge transfer resistance via modifying the composition of solid-electrolyte interphase. The resulting full cells with lithium iron phosphate cathodes exhibit a high specific capacity of ∼160 mAh/g, i.e., ∼0.6 mAh/cm 2 with excellent retention of 93.1 % at 120 cycles.
研究领域:
材料科学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 31
·20288-20299
·
IF 10.7
Liang Chai,Zhiheng Zou,Zhengsheng Yang,Guang Yang
Developing flexible polymer electrolytes that can concurrently promote ion conduction, uniform Li deposition, and robust solid electrolyte interphase (SEI) formation is promising for the development of next-generation lithium metal batteries (LMBs). Herein, a new polymeric zwitterionic electrolyte with a glass fiber support was investigated. A sulfobetaine zwitterionic crosslinker participated in in situ UV-triggered photopolymerization with a carbonate monomer and ether type dimethacrylate. The zwitterionic gel electrolyte (ZGE) demonstrated a high ionic conductivity exceeding 1 × 10−3 S cm−1 and electrochemical oxidative stability (>5 V vs. Li+/Li). The zwitterionic crosslinker in the ZGE was able to mediate homogeneous Li+ flux toward the lithium anode and suppress lithium dendrites (the Li/ZGE/Li cell can cycle stably for more than 1400 h with a current density of 0.1 mA cm−2). The ZGE also helped construct a LiF-rich SEI favorable for dendrite suppression. A Li/ZGE/LiFePO4 (LFP) cell demonstrated excellent long-term cycling stability (>600 cycles with a capacity retention of 92%, high discharge capacity of 155 mA h g−1, and coulombic efficiency of >99.5%). The ZGE could also support a Li/Ni0.815Co0.15Al0.035O2 (NCA) cell to operate with a high specific capacity of 232 mA h g−1. The flexible ZGE made it possible for a pouch-type Li/LFP cell to cycle and function well in a flat and bending state. This polymer electrolyte holds great promise for the exploration of high-energy polymeric LMBs.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）