ACS Applied Materials & Interfaces
·
2022
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IF 10.383
Zhichuan Shen,Jiawei Zhong,Shiyong Jiang,Wenhao Xie,Shiying Zhan,Kaiji Lin,Linyong Zeng,Hailing Hu,Guide Lin,Yuhan Lin,Shuhui Sun,Zhicong Shi
Because of their high ionic conductivity, utilizing gel polymer electrolytes (GPEs) is thought to be an effective way to accomplish high-energy-density batteries. Nevertheless, most GPEs have poor adaptability to Ni-rich cathodes to alleviate the problem of inevitable rapid capacity decay during cycling. Therefore, to match LiNi0.8Co0.1Mn0.1O2 (NCM811), we applied pentaerythritol tetraacrylate (PETEA) monomers to polymerize in situ in a polyacrylonitrile (PAN) membrane to obtain GPEs (PETEA-TCGG-PAN). The impedance variations and key groups during the in situ polymerization of PETEA-TCGG-PAN are investigated in detail. PETEA-TCGG-PAN with a high lithium-ion transference number (0.77) exhibits an electrochemical decomposition voltage of 5.15 V. Noticeably, the NCM811|PETEA-TCGG-PAN|Li battery can cycle at 2C for 120 cycles with a capacity retention rate of 89%. Even at 6C, the discharge specific capacity is able to reach 101.47 mAh g–1. The combination of LiF and Li2CO3 at the CEI interface is the reason for the improved rate performance. Moreover, when commercialized LFP is used as the cathode, the battery can also cycle stably for 150 cycles at 0.5C. PETEA and PAN can together foster the transportation of Li+ with the construction of a fast ion transport channel, making a contribution to stable charge–discharge of the above batteries. This study provides an innovative design philosophy for designing in situ GPEs in high-energy-density lithium metal batteries.
研究领域:
材料科学
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电化学
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电池技术
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高分子化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Pengcheng Li,Long Chen,Zuxin Wen,Daxu Zhang,Ying Zhang,Ning Zhang,Gen Chen,Xiaohe Liu
Lithium metal is recognized as the next generation anode material due to its ultra-high capacity. However, the safety hazards caused by the dendritic lithium growth hinder its practical application. In this work, rare earth nitrates, such as Y(NO 3 ) 3 , are introduced as electrolyte additives because of the unfixed coordination number and complex coordination configuration for rare earth cations. Molecular dynamics simulation reveals that the rare earth ion changes the solvation structure of the lithium ion. When it is combined with fluoroethylene carbonate (FEC), the interphase generated from electrochemical reactions is favorable for the dense Li deposition. As a result, a stable and high Coulombic efficiency is achieved for Li/Cu cells in commercial carbonate electrolyte with such additive. The Li/Li symmetrical cells can operate>1000 h at current density of 1 mA cm −2 . Moreover, the NCM811/Li full cells deliver superior cycling stability and better rate performance. This strategy sheds light on utilizing rare earth elements to optimize the electrolyte for lithium metal anode and it can be extended to other electrolytes aiming at sodium and potassium battery chemistry.
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
Advanced Science
·
2022
·Vol. 10
·期 3
·2203916
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IF 17.521
Jiazhu Guan,Xinping Feng,Qinghui zeng,Zhenfeng Li,Yu Liu,Anqi Chen,Honghao Wang,Wei Cui,Wei Liu,Liaoyun Zhang
Lithium metal batteries hold promise for energy storage applications but suffer from uncontrolled lithium dendrites. In this study, a new composite membrane based on modified natural polymer and ZIF-67 is designed and prepared by the in situ composite method for the first time. Among them, a modified natural polymer composed of lithium alginate (LA) and polyacrylamide (PAM) can be obtained by electrospinning. Importantly, the polar functional groups of natural polymers can interact by hydrogen bonding and MOFs can construct lithium-ion transport channels. Consequently, compared with LA-PAM electrolyte without MOF, the electrochemical stability window of ZIF-67-LA-PAM electrolyte becomes wider from 4.5 to 5.2 V, and the lithium-ion transference number ( t Li+ ) enhances from 0.326 to 0.627 at 30°C. It is worth noting that the symmetric cells with ZIF-67-LA-PAM have superior stable cycling performance at 40 and 100 mA cm −2 , and a high rate at 10C and 20C for LFP cells. Besides, the cell with NCM811 high-voltage cathode can run stably for 400 cycles with an initial discharge capacity of 136.1 mAh g −1 at 0.5C. This work provides an effective method for designing and preparing MOF-natural polymer composite electrolytes and exhibits an excellent application prospect in high-energy-density lithium metal batteries.
研究领域:
材料科学
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电化学
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储能技术
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电池技术
✓ 已验证
DOI
高影响因子
ChemSusChem
·
2024
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IF 7.5
Hui Chen,Yu-Xiang Xie,Long-Ji Dong,Hao Peng,Meng-Wei Lin,Miao-Lan Sun,Shi-Shi Liu,Jun-Bo Ma,Ling Huang,Shi-Gang Sun
Lithium-ion batteries, with high energy density and long cycle life, have become the battery of choice for most vehicles and portable electronic devices; however, energy density, safety and cycle life require further improvements. Single-functional group electrolyte additives are very limited in practical applications, a ternary polymer bifunctional electrolyte additive copolymer (acrylonitrile-butyl hexafluoro methacrylate- poly (ethylene glycol) methacrylate- methyl ether) (PMANHF) was synthesized by free radical polymerization of acrylonitrile, 2, 2, 3, 4, 4, 4-hexafluorobutyl methacrylate and poly (ethylene glycol) methyl ether methacrylate. A series of characterizations show that in Li metal anodes, the preferential reduction of PMANHF is conducive to the formation of a uniform and stable solid electrolyte interphase layer, and Li deposition is uniform and dense. At the NCM811 cathode, a film composed of LiF- and Li3N-rich is formed at the cathode-electrolyte interface, mitigating the side reaction at the interface. At 1.0 mA cm-2, the Li/Li cell can be stabilized for 1000 cycles. In addition, the Li/NCM811 cell can stabilize 200 cycles with a cathode capacity of 153.7 mAh g-1, with the capacity retention of 89.93%, at a negative/positive capacity ratio of 2.5. This study brings to light essential ideas for the fabrication of additives for lithium-metal batteries.
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
产品关联
DOI
PubMed
高影响因子
Journal of Energy Storage
·
2024
·
IF 8.9
Jian Ma,Yueyue Wu,Lei Dong,Mengyue Yu,Zhendong Zhu,Le Zhang,Linchao Zhang,Hongfa Xiang
Cathode–electrolyte integration via in-situ polymerization is an effective strategy to reduce interfacial resistance in solid-state/quasi-solid-state lithium batteries ; however, ion conduction in the fraction of polymer electrolyte is still to be enhanced. Herein, we demonstrate a separator-free cathode–electrolyte integrated structure employing a novel poly(di(ethylene glycol) ethyl ether acrylate)-based quasi-solid polymer electrolyte (LiTFSI-poly(DEGA)-FEC QSPE, denoted as PDEGA-QSPE), prepared via UV-assisted in-situ polymerization. Poly(DEGA) as a linear polymer contains abundant ethylene oxide (EO) segments in its branched chain, exhibiting excellent flexibility and high adhesion. Benefited from the flexible molecular structure, PDEGA-QSPE exhibits a glass transition temperature ( T g ) as low as around −68 °C and a good room-temperature ionic conductivity of 2.3 × 10 −4 S cm −1 , and it also shows an oxidative potential up to 4.7 V. The LiFePO 4 |PDEGA-QSPE|Li battery possesses an initial capacity of 149.2 mAh g −1 and a capacity retention of 92.5 % after 300 cycles at 0.2 C under room temperature, and poly(DEGA)-based QSPE also has the potential to be applied to the high-voltage NCM811||Li battery. Compared with widely-employed monomers for in-situ polymerization such as poly(ethylene glycol) diacrylate (PEGDA), poly(DEGA) possesses remarkably improved flexibility and ion conduction capability, exhibiting broad research and application prospects.
研究领域:
材料科学
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电化学
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能源存储
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电池技术
✓ 已验证
DOI
高影响因子
Materials Chemistry Frontiers
·
2023
·Vol. 7
·期 18
·4152-4163
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IF 7
Kun Yang,Zhichuan Shen,Junqiao Huang,Jiawei Zhong,Yuhan Lin,Junli Zhu,Jiashun Chen,Yating Wang,Tangtang Xie,Jie Li,Zhicong Shi
Gel polymer electrolytes (GPEs) have attracted substantial interest due to their high lithium-ion conductivities and safety. However, the narrow electrochemical stability windows and poor mechanical properties of conventional GPEs limit their application in batteries targeting high energy densities. Herein, a fluorine-modified acrylate-based GPE is designed and prepared via in situ polymerization, which exhibits a wide electrochemical window, high Li+ transference number and ionic conductivity. The introduced fluorine-rich group can promote the uniform deposition of Li ions and inhibit the growth of Li dendrites, thus enabling stable cycling of Li symmetric cells for 2400 h at 0.1 mA cm−2. Meanwhile, a Li-metal cell with the NCM811 cathode and GPE exhibits promising long-term cycling stability (91% capacity retention after 260 cycles, 2C) and rate capability (e.g., 125 mA h g−1 at 10C), when cycled between 3.0 and 4.5 V at 25 °C. Moreover, this GPE is also successfully utilized in pouch cells, and 81% capacity is maintained after 150 cycles. This study demonstrates the potential of fluorination in promoting the performance of GPEs and can serve as a guideline for the future development of Li-metal batteries with high-nickel layered cathode materials.
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
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
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IF 19
Yaxin Zhang,Tongshuai Wang,Jiawen Tang,Yunsong Li,Yuxiang Guo,Lu Cheng,Jiacheng Liu,Ahu Shao,Chunwei Li,Zhiqiao Wang,Xiaoyu Tang,Yisheng Hu,Yue Ma
The paradigm shift toward the disposal of retired batteries demands sustainable and cost-effective recycling methods that surpass conventional pyro-/hydrometallurgy-based techniques, offering superior profitability, energy efficiency, resource utilization, and environmental benefits. In this study, a one-step modulation approach is presented for regenerating spent Ni-rich layered oxides featured with exceptional ion diffusivity and high-temperature stability. By exploiting decomposed species from Li 6 Zr 2 O 7 , monitored via high-temperature X-ray diffraction, the strategy simultaneously enables: Li source replenishment, Zr doping into the bulk lattice, and Conformal ion-conductive Li 2 ZrO 3 coating on regenerated LiNi 0.8 Co 0.1 Mn 0.1 O 2 (R-NCM811-2%LZO). Crucially, the upcycling process strategically utilizes lattice vacancies in the oxide to facilitate Zr dopant diffusion, while Li 2 ZrO 3 coating elevates corrosion resistance and thermal stability. Operando phase tracking reveals that the regenerated cathode maintains reversible lattice breathing and undergoes a continuous, kinetics-boosted phase transition. By pairing R-NCM811-2%LZO cathode with graphite anode in a 3.0 Ah pouch-format cell, the prototype achieves an energy density of 302 Wh kg −1 , extreme power output of 1260 W kg −1 , 63% mitigation of self-discharge rate at 55 °C, as well as robust cycling across a wide temperature range. This value-added strategy upgrades spent NCM811 into high-temperature-tolerant, fast-charging cathodes, paving the way for sustainable battery recycling and circular economy initiatives.
研究领域:
材料科学
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电化学
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储能技术
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电池回收
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纳米技术
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环境科学
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固态化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2022
·
IF 9.794
Shijie Lu,Xiaorong Chu,Chunli Li,Zhikun Zhao,Jianxiong Xiao,Borong Wu,Daobin Mu
High ionic conductivity and good interface compatibility have always been two major bottlenecks for solid-state electrolytes. Herein, a composite electrolyte membrane comprising poly (propylene carbonate), PVDF-HFP and Li 6 · 3 La 3 Zr 1 · 4 Ta 0 · 6 O 12 is successfully prepared via electrospinning. With the assistance of succinonitrile, the synthesized solid-state electrolyte exhibits high ionic conductivity (1.32 × 10 −3 S cm −1 at room temperature), oxidation potential up to 4.5 V vs Li/Li + and high Li + transference number (0.81). This desirable performance is attributed to the combination of PPC with good Li + conduction ability and PVDF-HFP with excellent mechanical properties, forming a continuous transport framework within the electrolyte. The introduced active fillers and small molecular additive not only benefit to fast Li + mobility, but also reinforce the stability towards Li metal. Li symmetric cell using the solid-state electrolyte can last for 800 h at a current density of 1.0 mA cm −2 with a low overpotential. The NCM811 cell using the electrolyte membrane shows high initial discharge specific capacity (184.3 mAh g −1 at 1 C) and good capacity retention (80.1% after 300 cycles at 30 °C).
研究领域:
材料科学
·
电化学
·
电池技术
·
纳米技术
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2023
·
IF 9.2
Yuhan Lin,Zhichuan Shen,Junqiao Huang,Junli Zhu,Shiyong Jiang,Shiying Zhan,Yu Xie,Jiahong Chen,Zhicong Shi
Gel polymer electrolytes (GPEs) play a crucial role in promoting the development of lithium metal batteries , as they combine the high ionic conductivity of liquid electrolytes with the enhanced safety provided by solid electrolytes . However, traditional polymer electrolytes are typically poured using non-in-situ methods, which results in poor electrode-electrolyte contact and compromises their performance. In this paper, in situ thermal polymerization is utilized to incorporate di-pentaerythritol pentaacrylate (DPPA) and 3,3,4,4,5,5,6,6,7,7,8,8-tridecafluorooctyl acrylate (TFOA) into PAN spinning porous membranes. Application of TFOA reduces the crystallinity of GPEs and thus enhancing the Li + transport capability, which enables the newly constructed GPEs to exhibit an ionic conductivity of 2.52 × 10 −3 S cm −1 and a lithium-ion transport number of 0.61 at 30 °C. Simultaneously, fluoro-containing groups actively contribute to the formation of a negative solid electrolyte interphase (SEI) film full of LiF, ensuring the stable operation of Li symmetrical batteries for over 2000 h at a current density of 0.40 mA cm −2 . The capacity retention rate of lithium metal batteries (LMBs) with commercial NCM811 cathodes reaches 88.2% after 300 cycles. We firmly believe that our newly designed gel polymer electrolytes (GPEs) can offer a viable solution for high-voltage and high-rate LMBs.
研究领域:
材料科学
·
电化学
·
电池技术
·
聚合物化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）