MACROMOLECULES
·
2023
·
IF 5.5
Jirong Wang,Chi Zhang,Yong Zhang,Gong Chen,Rinaldo Poli,Xiaolin Xie,Zhigang Xue
Assembling polymer electrolytes (PEs) with lithium metal anodes is a promising strategy to address safety and specific capacity concerns. Molecular design on conductive polymer matrices avoids inherent high crystallinity, poor ion transport, and combustion drawbacks by adjusting the chain structure and functional groups. However, conventional structural modulation methods are difficult to conduct via in situ polymerization and cell assembly, thus hampering the further performance enhancement of PEs in lithium batteries. Herein, we report a simple aza-Michael addition method induced by lithium salts for designing and fabricating high-performance PEs. This method fulfills the in situ structure modulation of polyether-based PEs without any introduction of non-electrolytic components. The obtained polyether electrolytes exhibit a more amorphous cross-linked structure, leading to a favorable medium for ion migration and excellent flexibility. In addition, the introduction of C–N bonds imparts excellent non-flammability to the material as well as the ability to interact with sulfolane. Hence, the in situ-constructed gel polymer electrolyte (GPE) is characterized by a high ionic conductivity (1.76 × 10–4 S cm–1 at 30 °C) and excellent interface stability with the electrodes. The assembled Li/LiFePO4 (LFP) battery based on this newly designed GPE exhibits a high initial specific discharge capacity and a good rate performance (112.7 mAh g–1 at 5 C). Long-term stability was also demonstrated, with a capacity retention of 86.8% after 500 cycles at 0.5 C.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Advanced Energy Materials
·
2018
·Vol. 8
·期 36
·1802176
·
IF 21.875
Xiaoyu Jiang,Xingwei Liu,Ziqi Zeng,Lifen Xiao,Xinping Ai,Hanxi Yang,Yuliang Cao
Dual-carbon batteries provide a new perspective on energy storage technology due to their high voltage and low cost. Herein, a novel Na + -based dual-carbon battery (Na + -DCB) is developed based on a nonflammable trimethyl phosphate (TMP) electrolyte with sodium bis(trifluoromethanesulfonate)imide salt (NaTFSI). As the molar ratio of NaTFSI/TMP increases to 1:2, the graphite cathode shows a high reversible capacity of 52.9 mAh g −1 , excellent rate capability (21.0 mAh g −1 at 2000 mA g −1 ) and superstability cycling performance (≈100% capacity retention after 750 cycles). In addition, a stable solid electrolyte interface (SEI) film is formed on the surface of hard carbon anode by the preferential reductive decomposition of TFSI − , which suppresses decomposition of TMP. In this case, the Na + -DCB is capable to provide an operation voltage of 4.0 V and excellent electrochemical performance. This work provides new insights for developing new dual-carbon batteries with safety, low cost, and absence of heavy metals.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 23
·12575-12587
·
IF 14.511
Dichang Guan,Guorong Hu,Zhongdong Peng,Yanbing Cao,Jiahui Wu,Min Huang,Shuai Zhang,Yuqing Dai,Yifan Gong,Ke Du
In this work, we develop a nonflammable low-concentration electrolyte (LCE) based on the Li+-solvation sheath structure. It consists of only 0.4 M LiPF6 in the mixture of ethylene carbonate (EC), dimethyl carbonate (DMC), and 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE). Abundant incombustible TTE is used as an inert cosolvent to regulate the Li+-solvation sheath structure. With the addition of TTE, the oxidation stability of the LCE is enhanced as a result of reduced free-state solvent molecules and strengthened interactions between Li+ and EC/DMC molecules. The rate and cycling performances of Li‖LFP and Li‖NCM811 cells in 0.4 M LiPF6–EC/DMC/TTE (1 : 1 : 4, v/v/v) (0.4 M-114) are much better than in 0.4 M LiPF6–EC/DMC (1 : 1, v/v), and even better than in the conventional electrolyte (1 M LiPF6–EC/DMC (1 : 1, v/v)). The graphite‖LiNi0.5Co0.2Mn0.3O2 (NCM523) pouch cells using the 0.4 M-114 electrolyte show excellent cycling and safety performances, demonstrating the feasibility of using the nonflammable LCEs in practical applications. This work provides a nonflammable low-concentration electrolyte for lithium-ion batteries (LIBs) and provides a new insight into the development of electrolytes for LIBs.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2020
·Vol. 167
·期 9
·090520
·
IF 3.721
Huiying Liang,Xiaoxi Zuo,Lengdan Zhang,Wenda Huang,Qiuyu Chen,Tianming Zhu,Jiansheng Liu,Junmin Nan
Developing a nonflammable electrolyte is an efficient strategy to eliminate fire hazards and improve battery safety. Electrolytes containing nonflammable phosphate solvents enhance battery safety to a certain extent, but their compatibility with electrodes remains an obstacle. Here, a nonflammable electrolyte based on carbonate solvent is designed to resolve this dilemma while guaranteeing battery performance. We demonstrate that a nonflammable electrolyte employing the popular film-forming solvent ethylene carbonate (EC) and 1,2-dimethoxyethane (DME) with 2.3 mol kg−1 lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) has excellent thermal stability owing to the unique solution molecule structure. What's more, the nonflammable electrolyte possesses excellent compatibility with both LiNi0.6Co0.2Mn0.2O2 and graphite electrode. The initial specific capacity and capacity retention rate of graphite/LiNi0.6Co0.2Mn0.2O2 punch cells employing this electrolyte are 169.3 mAh g−1 and 98.7% (after 50 cycles), respectively, which are comparable to those of cells employing traditional carbonate electrolytes. Besides, short-circuit test of the pouch cell suggests that the release of gases accompanied by decomposition of electrolyte under abuse conditions is effectively suppressed. All of these results show a promising prospect of this nonflammable electrolyte for application in high-safety Li-ion batteries.
研究领域:
材料科学
·
能源技术
✓ 已验证
DOI
高影响因子
ChemElectroChem
·
2019
·Vol. 6
·期 4
·1229-1234
·
IF 3.975
Xiao-Min Zhao,Yong-Wang Yan,Xiao-Xia Ren,Liang Chen,Shou-Dong Xu,Shi-Bin Liu,Xiao-Min Wang,Ding Zhang
Graphical Try to set the night on fire : a nonflammable electrolyte for room-temperature sodium-sulfur (RT Na-S) batteries is prepared by introducing trimethyl phosphate (TMP) into 1.0 M NaClO 4 -ethylene carbonate/ propylene carbonate (EC/PC) electrolyte. With 15 wt.% TMP-contained electrolyte the C/S electrode shows excellent cycling stability with a reversible capacity of 788 mAh g −1 after 80 cycles as well as a good rate performance. To address the safety concern for room-temperature sodium-sulfur batteries, such as fires easily triggered by organic electrolytes, an applicable non-flammable electrolyte formula was developed by introducing trimethyl phosphate (TMP) into 1.0 M NaClO 4 -ethylene carbonate/propylene carbonate electrolyte. It is demonstrated that the electrolyte containing 15 wt.% TMP was a optimized formula, exhibiting nonflammability, thermal stability, electrochemical compatibility and lasting cell performance. Using this optimized electrolyte formula, the sulfur cathode exhibited a stable capacity of 788 mAh g −1 at a rate of 0.1 C and excellent rate capability of 441 and 177 mAh g −1 for 200 cycles at rates of 1 C and 5 C , respectively. When the TMP content further increases to 25 wt.%, the specific capacity of batteries declined significantly due to unstable SEI. Our study can shed light on the development of flame-retardant electrolyte for room-temperature sodium-sulfur or other batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
·
2024
·
IF 14
Zhiwen Deng,Ye Jia,Yan Deng,Changhaoyue Xu,Xuemei Zhang,Qiujie He,Jianan Peng,Hao Wu,Wenlong Cai
High-voltage battery systems bring significant increases in energy density but are also accompanied by fast degradation of electrochemical performance and serious safety issues. Herein, Li + coordination structure regulation was conducted to formulate a non-flammable electrolyte, which consists of 1.5 M lithium bis (fluor sulfonyl) imide (LiFSI) in triethyl phosphate and methyl 2,2,2-trifluoromethyl carbonate (FEMC). The renamed TEP-FEMC-FEC (TFF) electrolyte exhibits an FSI − -dominated solvation structure contributed by the weakly-solvating ability of FEMC. The generated inorganic-rich interfacial layers are conducive to stabilizing the phase transition of high-voltage cathodes while suppressing the dendritic growth on lithium metal or co-intercalation behavior in graphite anode. This TFF electrolyte enables LiCoO 2 || Li batteries to achieve capacity maintenance over 79% after 400 cycles with high-rate of 5 C at an ultra-high voltage of 4.6 V, and an outstanding capacity exceeding 100 mA h g − 1 even at a super-high current density of 20 C. Additionally, the Ah-level LiCoO 2 || graphite pouch cells also exhibit high capacity retention and satisfactory safety performance even under fast charging. This work provides a novel research direction for the pursuit of high energy density non-flammable electrolytes.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
FIRE TECHNOLOGY
·
2019
·Vol. 56
·期 6
·2349-2364
·
IF 1.42
Zheng Hao,Fang Wei,Sun Yi,Liang Xin,Xiang Hongfa,Jiang Lihua,Wang Qingsong
Nonflammable electrolytes are promising substitutes for the state-of-the-art carbonate-based electrolytes in order to directly enhance the safety characteristics of lithium ion batteries. Combination of trimethyl phosphate (TMP) and a fluorinated ether of 1,1,2,2-tetrafluoroethyl 2,2,3,3-tetrafluoropropyl ether (FEPE) is designed to formulate nonflammable electrolytes. The reformulated electrolytes of 1 mol/L LiPF 6 /TMP + FEPE (9:1, 8:2 and 7:3, w/w) are totally nonflammable. The FEPE solvent has higher oxidative stability and the FEPE-containing electrolytes have better separator wettability than the pure TMP electrolyte (1 mol/L LiPF 6 /TMP). The improved oxidative stability and separator wettability can enhance electrochemical stability of electrolyte on high-voltage cathode LiNi 0.5 Mn 1.5 O 4 . In Li 4 Ti 5 O 12 /LiNi 0.5 Mn 1.5 O 4 cells, the FEPE-containing electrolyte exhibits the better cycling stability than the pure TMP electrolyte, and the solvent composed of TMP + FEPE (8:2) is the optimal ratio. The Li 4 Ti 5 O 12 /LiNi 0.5 Mn 1.5 O 4 cell with the optimal electrolyte exhibits better rate capability because of the reduced polarization and improved oxidation stability. This work reveals the effect of fluorinated ethers on separator wettability of TMP-based nonflammable electrolytes and high-voltage applications.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Ge Zhang,Sunfa Wang,Kanghou Ma,Caiyue Sun,Chen Wang,Fangshuo Zhou,Xinyue Zhao,Xiqiang Huang,Zhiguo Liu,Ningning Wu,Yaohui Zhang
Dual ion batteries, which have emerged as a novel energy storage device in recent years, are highly valued for their high operating voltage, safety, and environmental friendliness, attracting significant attention. However, the safety characteristics of these batteries are greatly reduced due to the high flammability of conventional carbonate-based electrolytes. The development of a non-flammable electrolyte with high safety and excellent reversible plating/stripping characteristics is crucial for the advancement of potassium (K) −based dual ion batteries. Compared to high concentration electrolytes, the use of low electrolyte concentration limits the capacity derived from anion intercalation into the graphite layers. In this work, a 3.75 M KFSI/TEP:DMC (2:1 v/v) electrolyte was configured using non-flammable triethyl phosphate (TEP) as the main solvent, dimethyl carbonate (DMC) as the co-solvent, and potassium bis(fluorosulfonyl)imide (KFSI) as the salt. This electrolyte not only exhibits highly non-flammable properties but also demonstrates excellent plating/stripping reversibility in K||Al half batteries, achieving an average coulombic efficiency of ∼ 98.9 % over 1200 cycles. Furthermore, long-term reversibility tests conducted with K||K symmetric batteries indicate a cycle life exceeding 6000 h, which corresponds to more than 250 days of continuous operation. In conclusion, we assembled a K-based anode-free dual ion battery, with aluminum serving as the anode and graphite as the cathode, which exhibited an exceptional cyclic lifespan. At 0.2 A g −1 , the battery demostrated stable cycling for over 200 cycles, maintaining a capacity retention rate of 100 %. This research paves the way for the development of high-safety K-based anode-free dual ion batteries.
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
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Jiaqing Jiang,Yiting Lin,Haipeng You,Menglei Yao,Jie Sun,Long Chen,Chunzhong Li
With the rapid evolution of electric vehicles, there is a growing demand for batteries with high energy and safety. Among various options, the LiNi0.5Mn1.5O4 (LNMO)/phosphorus battery has emerged as one of the most promising candidates due to its appropriate lithiation potential and remarkable specific capacity. However, challenges related to high-voltage, polyphosphate dissolution, and phosphorus combustion safety issues persist in this system. Herein, we design a nonflammable electrolyte with a wide electrochemical window of over 5.8 V. It successfully mitigates the shuttling effect observed in phosphorus anodes, resulting in an impressive capacity retention of 80% over 600 cycles. The LNMO||P/C full cell delivers a stable capacity of 97.5 mAh g–1 over 200 cycles with an exceptional energy density of 350 Wh kg–1. These findings mark a significant step forward in the development of high-safety and high-performance phosphorus anode batteries, opening up exciting possibilities for their application in electric vehicles and beyond.
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 Communications
·
2021
·Vol. 12
·期 1
·1-13
·
IF 14.919
Wu Junru,Wang Xianshu,Liu Qi,Wang Shuwei,Zhou Dong,Kang Feiyu,Shanmukaraj Devaraj,Armand Michel,Rojo Teofilo,Li Baohua,Wang Guoxiu
The current Li-based battery technology is limited in terms of energy contents. Therefore, several approaches are considered to improve the energy density of these energy storage devices. Here, we report the combination of a heteroatom-based gel polymer electrolyte with a hybrid cathode comprising of a Li-rich oxide active material and graphite conductive agent to produce a high-energy “shuttle-relay” Li metal battery, where additional capacity is generated from the electrolyte’s anion shuttling at high voltages. The gel polymer electrolyte, prepared via in situ polymerization in an all-fluorinated electrolyte, shows adequate ionic conductivity (around 2 mS cm −1 at 25 °C), oxidation stability (up to 5.5 V vs Li/Li + ), compatibility with Li metal and safety aspects (i.e., non-flammability). The polymeric electrolyte allows for a reversible insertion of hexafluorophosphate anions into the conductive graphite (i.e., dual-ion mechanism) after the removal of Li ions from Li-rich oxide (i.e., rocking-chair mechanism).
研究领域:
材料科学
·
能源存储技术
✓ 已验证
DOI
PubMed
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
·
2019
·
IF 0
Junxiong Wu,Jiapeng Liu,Ziheng Lu,Kui Lin,Yu-Qi Lyu,Baohua Li,Francesco Ciucci,Jang-Kyo Kim
Room temperature (RT) sodium-sulfur (Na-S) batteries are a promising technology for stationary energy storage thanks to their high energy density of 1274 Wh kg −1 and low cost. However, RT Na-S batteries are hazardous because they use highly volatile and flammable electrolytes. Here, we develop a new nonflammable electrolyte for RT Na-S batteries, consisting of sodium trifluoromethanesulfonimide (NaTFSI) in a mixture of trimethyl phosphate (TMP) and fluoroethylene carbonate (FEC). The nonflammable electrolyte facilitates highly stable and reversible Na plating/stripping during cycles. The dendrite-free Na-S battery with the NaTFSI/TMP+FEC electrolyte delivers a remarkable reversible capacity of 788 mAh g −1 after 300 cycles at 1C, corresponding to a negligible capacity decay below 0.04% per cycle. The ab initio molecular dynamics simulations and surface analysis reveal the formation of a NaF-rich solid electrolyte interphase (SEI) film with reduced interfacial resistance thanks to the introduction of FEC into the electrolyte. The formed NaF SEI layer suppresses the growth of Na dendrites on the anode, enhancing the electrochemical performance of the RT Na-S batteries. The new findings reported here will shed new light on dendrite-free RT Na-S batteries by the rational design of nonflammable electrolytes.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
DOI
危险品化学品经营许可证（带存储）