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
·
能源技术
✓ 已验证
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
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Yaqi Li,Pengjian Zuo,Ruinan Li,Hua Huo,Yulin Ma,Chunyu Du,YunZhi Gao,Geping Yin,Robert S. Weatherup
Rechargeable Mg-ion batteries typically suffer from either rapid passivation of the Mg anode or severe corrosion of the current collectors by halogens within the electrolyte, limiting their practical implementation. Here, we demonstrate the broadly applicable strategy of forming an artificial solid electrolyte interphase (a-SEI) layer on Mg to address these challenges. The a-SEI layer is formed by simply soaking Mg foil in a tetraethylene glycol dimethyl ether solution containing LiTFSI and AlCl3, with Fourier transform infrared and ultraviolet–visible spectroscopy measurements revealing spontaneous reaction with the Mg foil. The a-SEI is found to mitigate Mg passivation in Mg(TFSI)2/DME electrolytes with symmetric cells exhibiting overpotentials that are 2 V lower compared to when the a-SEI is not present. This approach is extended to Mg(ClO4)2/DME and Mg(TFSI)2/PC electrolytes to achieve reversible Mg plating and stripping, which is not achieved with bare electrodes. The interfacial resistance of the cells with a-SEI protected Mg is found to be two orders of magnitude lower than that with bare Mg in all three of the electrolytes, indicating the formation of an effective Mg-ion transporting interfacial structure. X-ray absorption and photoemission spectroscopy measurements show that the a-SEI contains minimal MgCO3, MgO, Mg(OH)2, and TFSI–, while being rich in MgCl2, MgF2, and MgS, when compared to the passivation layer formed on bare Mg in Mg(TFSI)2/DME.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Polymers
·
2019
·Vol. 11
·期 8
·1306
·
IF 3.164
Shiqi Wang,Chun Wei,Wenwen Ding,Linmin Zou,Yongyang Gong,Yuanli Liu,Limin Zang,Xu Xu
A high-voltage electrolyte can match high-voltage positive electrode material to fully exert its capacity. In this research, a sulfolane plasticized polymer electrolyte was prepared by in situ photocuring. First, the effect of the sulfolane content on the ionic conductivity of the gel polymer electrolyte was investigated. Results showed that the ionic conductivity variation trend was in good agreement with the exponential function model for curve fitting. Second, the activation energy was calculated from the results of the variable temperature conductivity tests. The activation energy was inversely proportional to the sulfolane content. For the sulfolane content of 80 wt. % in gel polymer electrolyte (GPE)-80 (19.5 kJ/mol), the activation energy was close to conventional liquid electrolyte (9.5 kJ/mol), and the conductivity and electrochemical window were 0.64 mS/cm and 5.86 V, respectively. The battery cycle performance test showed that the initial specific discharge capacities of GPE-80 and liquid electrolyte were 176.8 and 148.3 mAh/g, respectively. After 80 cycles, the discharge capacities of GPE-80 and liquid electrolyte were 115.8 and 41.1 mAh/g, and the capacity retention rates were 65.5% and 27.7%, respectively; indicating that GPE-80 has a better specific discharge capacity and cycling performance than the liquid electrolyte. SEM images indicated that GPE-80 can suppress the growth of lithium dendrites. The EDS test showed that GPE-80 can inhibit the dissolution of metal ions in the cathode material.Keywords:lithium battery;sulfolane;gel polymer electrolyte;high-voltage electrolyte;UV curable
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2018
·
IF 0
Yumei Zhou,Jianchen Hu,Peixin He,Yuhong Zhang,Jingjing Xu,Xiaodong Wu
Imide salt–polymer plastic crystal electrolytes (PPCEs) have been demonstrated to be very promising solid-state electrolytes for ambient lithium ion batteries (LIBs). However, anodic Al dissolution at high voltage, due to these salts, cannot form an AlF3/LiF passivation film (like LiPF6) on an Al surface, which limits their application in high-voltage solid-state LIBs. In this work two ambient workable PPCEs with different lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) concentrations are designed to investigate anodic Al dissolution suppression in solid-state imide salt-based electrolytes. The anodic Al dissolution is examined by a scanning electron microscope (SEM) and an energy dispersive spectrometer (EDS). The electrochemical performance is evaluated by solid-state LiCoO2/PPCE/Li4Ti5O12 cells. The results demonstrate that anodic Al dissolution is efficiently suppressed and the cell electrochemical performance is greatly elevated by optimizing LiTFSI concentration in PPCEs. The suppression mechanism of Al corrosion in concentrated PPCE is analyzed and suggested.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Rupeng Zhang,Can Cui,Ruinan Li,Yaqi Li,Chunyu Du,Yunzhi Gao,Hua Huo,Yulin Ma,Pengjian Zuo,Geping Yin
Due to the good safety and high energy density , rechargeable Mg-metal batteries (RMMBs) have been regarded as a potential competitor of Li-metal batteries (LMBs). However, the Mg(TFSI) 2 -based conventional electrolytes will cause large overpotential in reversible plating/stripping attributed to the high ion transport impedance of the electrolyte decomposition products. Here, an artificial interphase composed of amorphous (a-) MgCl 2 @polymer on the Mg-metal surface is prepared by in-situ chemical reaction of metallic Mg with H 3 PO 4 and SiCl 4 in sequence, and can effectively inhibit the electrolyte decomposition and facilitate Mg 2+ transport, which plays the role of solid electrolyte interface (SEI) on Mg anode. The Mg-Mg symmetrical cell with modified Mg electrode exhibits lower overpotential (~0.25 V) and interfacial impedance than bare Mg electrode in 0.5 M Mg(TFSI) 2 /DME electrolyte. The voltage hysteresis in the Mg-S and Mg-Mo 6 S 8 batteries with the modified Mg anode is greatly improved compared to bare Mg anode. This work provides a new idea for future applications of passivation-free Mg-metal anode technology in the MMBs based on conventional electrolytes.
研究领域:
材料科学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
Nature Energy
·
2024
·
IF 49.7
Li Siyuan,Zhang Jiahui,Zhang Shichao,Liu Qilei,Cheng Hao,Fan Lei,Zhang Weidong,Wang Xinyang,Wu Qian,Lu Yingying
High-performance, cost-efficient electrolyte systems are sought after for high-energy-density multivalent metal batteries. However, the expensive precursor and complex synthesis process hinders exploration of cathode electrode/electrolyte interfaces and solvation structures. Here we developed a universal cation replacement method to prepare low-cost, high-reversibility magnesium and calcium electrolytes derived from a zinc organoborate solvation structure. By rationally adjusting the precursor chain length and F-substitution degree, we can fine tune anion participation in the primary solvation shell. A completely dissociated Mg organoborate electrolyte enables high current endurance and enhanced electrochemical kinetics, whereas the Ca organoborate electrolyte with strong coordination/B–H inclusion offers a stable solid–electrolyte interphase with high coulombic efficiency. A rechargeable 53.4 Wh kg −1 Mg metal prototype is achieved with a 30 μm Mg anode, a low electrolyte/sulfur ratio (E/S = 5.58 μl mg −1 ) and a modified separator/interlayer. This work provides innovative strategies for reversible electrolyte systems and high-energy-density multivalent metal batteries.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Peng Cui,Tiantian Wang,Zihan Wang,Heshun Geng,Pengcheng Song,Fang Hu,Junhua You,Kai Zhu
The progress of rechargeable zinc (Zn) ion batteries (RZBs) has been significantly impeded by the occurrence of side reactions and dendritic issues on Zn anodes, which are attributed to the intricate reaction kinetics observed in aqueous electrolytes. Herein, we propose a co-solvent electrolyte comprising a combination of N, N-dimethylformamide (DMF) and Dimethyl sulfoxide (DMSO). This electrolyte reconstructs the surface of the Zn anode and generates a dense and robust solid electrolyte interface (SEI), which promotes uniform Zn 2+ deposition and enhances Zn 2+ transport kinetics. The DFT further shows that the electrolyte has a unique solvated structure which enables uniform Zn 2+ deposition and the creation of stable SEI. By utilizing these advantages, the co-solvent electrolyte is capable of enduring uninterrupted cycling for more than 4000 h at a current density of 1 mA cm −2 , and for over 2000 h at a current density of 5 mA cm −2 . Furthermore, the Zn||NH 4 V 4 O 10 full cell demonstrated exceptional electrochemical performance with regard to charge/discharge capacity and cycle stability. This study showcases the effectiveness of non-aqueous electrolytes, which will enable the progress of secure and high-capacity RZBs.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
Advanced Energy and Sustainability Research
·
2021
·Vol. 3
·期 1
·2100140
·
IF 0
Junhua Zhou,Xueyu Lian,Qitao Shi,Yu Liu,Xiaoqin Yang,Alicja Bachmatiuk,Lijun Liu,Jingyu Sun,Ruizhi Yang,Jin-Ho Choi,Mark H. Rummeli
Although lithium (Li) metal anode/lithium–manganese-rich (LMR) cathode batteries have an ultrahigh energy density, the highly active Li metal and structural deterioration of LMR can make the usage of these batteries difficult. Herein, a multifunctional electrolyte containing LiBF 4 and LiFSI dual-salt additives is designed, which enables the superior cyclability of Li/LMR cells with capacity retentions of ≈83.4%, 80.4%, and 76.6% after 400 cycles at 0.5, 1, and 2 C, respectively. The dual-salt electrolyte can form a thin, uniform, and inorganic species-rich solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI). In addition, it alleviates the bulk Li corrosion and enhances the structural sustainability of LMR cathode. Moreover, the electrolyte design strategy provides insights to develop other high-voltage lithium metal batteries (HVLMBs) to enhance the cycle stability.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
ACS Applied Energy Materials
·
2025
·
IF 5.5
Yilong Lin,Yanshan Ji,Shuqing Gao,Sheng Huang,Jiawei Li,Wenyang Zhang,Qi Peng,Feng Liu,Yanwu Chen,Yuezhong Meng
In lithium (Li)-metal batteries (LMBs), the functional electrolytes need to be compatible with both a high-voltage cathode and a highly reactive anode. However, the carbonate-based electrolytes in commercial lithium-ion batteries (LIBs) exhibit insufficient reductive stability due to severe side reactions and the formation of lithium dendrites on the Li anode. In this study, the use of LiPF6 and lithium difluorobis(oxalato) phosphate (LiDFBOP) dual-salt electrolyte composed of ester and ether cosolvents (FEC/DME) enables the stabilization of the high-voltage LMBs through modulating the interfacial electrochemistry. Such an electrolyte design strategy is demonstrated to regulate the Li plating/stripping behavior by forming a robust anion-derived solid electrolyte interphase (SEI) film on the anode and to improve the cathode/electrolyte interfacial stability under high-voltage conditions. As a result, the as-developed electrolyte exhibits stable cycling over 800 h in Li∥Li symmetric cells and ultralong lifespans with capacity retention of 66% after 2000 cycles in Li∥LiFePO4. Targeted electrolyte engineering is presented as a promising approach for practical high-performance Li-metal batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Energy Storage Materials
·
2023
·
IF 20.4
Xiaojuan Chen,Yan Meng,Dan Xiao,Yiying Wu,Lei Qin
Although metallic potassium or graphite anode with low redox potentials are desirable for potassium-ion batteries (PIBs), the severe capacity decay caused by consecutive reduction reactions on the aggressively reactive anode surface is inevitable because of the scarcity of an effective passivation layer. Additionally, the development of PIBs faces potential safety hazards due to the usage of reactive anodes with flammable electrolytes. Herein, a fire-retardant localized high-concentration electrolyte (LHCE) is formulated by adding a low-polarity co-solvent of highly fluorinated ether into the concentrated potassium bis(fluorosulfonyl)imide/trimethyl phosphate. A unique electrolyte solvation environment with the enhanced anion-cation interaction in an LHCE facilitates a durable anion-derived solid electrolyte interphase (SEI) with self-accelerated interfacial kinetics and minimizes the SEI dissolution compared to the conventional carbonate-based electrolyte. Consequently, the unmodified Al substrate could sustain stable potassium metal cycling above 3400 h (over 800 cycles) with high reversibility (98%), and the graphite anode retains prolonged cyclic stability (over 300 cycles) with a high reversible capacity (257.6 mAh g −1 ) and capacity retention (92.6 % at 0.2 C). Meanwhile, Al corrosion at high voltage is significantly suppressed, and the electrochemical window is extended due to less free solvents in an LHCE, enabling good electrolyte compatibility with high-voltage cathodes. Coupling non-flammable solvents and the concept of LHCE could facilitate a better understanding of electrolyte chemistry and offer more opportunities to use K or graphite anode for all Al substrate-based PIBs highlighted with high performance and superb safety.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Energy Storage Materials
·
2022
·
IF 20.831
Boheng Yuan,Bin Zhao,Qi Wang,Yuge Bai,Zhiwei Cheng,Zhi Cong,Yafei Lu,Fangdi Ji,Fei Shen,Peng-Fei Wang,Xiaogang Han
Researchers pursue mass production of thin solid electrolytes with high room-temperature (RT) conductivity for solid state batteries with high energy and safety. A novel solid-state composite polymer electrolyte (CPE) with high room-temperature conductivity is obtained by UV-polymerization method and applied for solid-state Li-metal batteries. A commercial PE separator is used as a framework to straighten the CPE. The thickness of this CPE is only 16 µm, which is consist with the thickness of the PE film. It shows a high ionic conductivity of 1.11 × 10 −4 S cm −1 at RT. Li//Li cell can stably cycle for more than 1000 h at 0.1 mA cm −2 current density at RT, and LiCoO 2 //Li solid-state batteries possess excellent rate performance and cycling stability with a capacity retention of 76.1% after 385 cycles from 145.3 mAh g −1 to 110.6 mAh g −1 with a 0.2 C rate at RT.
研究领域:
材料科学
·
能源技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）