Advanced Science
·
2021
·Vol. 8
·期 15
·2003241
·
IF 16.806
Shengzhao Zhang,Taibo Liang,Donghuang Wang,Yanjun Xu,Yongliang Cui,Jingru Li,Xiuli Wang,Xinhui Xia,Changdong Gu,Jiangping Tu
An elastic and safe electrolyte is demanded for flexible batteries. Herein, a stretchable solid electrolyte comprised of crosslinked elastic polymer matrix, poly(vinylidene fluoride-hexafluoropropylene) (PVDF-HFP), and flameproof triethyl phosphate (TEP) is fabricated, which exhibits ultrahigh elongation of 450%, nonflammability and ionic conductivity above 1 mS cm −1 . In addition, in order to improve the interface compatibility between the electrolyte and Li anode and stabilize the solid-electrolyte interphase (SEI), a protecting layer containing poly(ethylene oxide) (PEO) is designed to effectively prevent the anode from reacting with TEP and optimize the chemical composition in SEI, leading to a tougher and more stable SEI on the anode. The LiFePO 4 /Li cells employing this double-layer electrolyte exhibit an 85.0% capacity retention after 300 cycles at 1 C. Moreover, a flexible battery based on this solid electrolyte is fabricated, which can work in stretched, folded, and twisted conditions. This design of a stretchable double-layer solid electrolyte provides a new concept for safe and flexible solid-state batteries.
研究领域:
材料科学
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电化学
·
储能技术
·
高分子科学
·
锂电池
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2024
·
IF 5.4
Ruliang Liu,Shimei Song,Jiaqi Xue,Huiping Deng,Suixiang Li,Qingwei Cheng
Lithium metal anodes are promising candidates for next-generation high-energy density batteries. Unstable lithium–electrolyte interfaces caused by uncontrolled dendrite growth and side reactions still hinder its practical process. In this work, an all-organic solid electrolyte interphase (SEI) film coupling hardness with softness has been prepared to achieve a dendrite-free lithium metal anode by designing polymer brushes rationally (poly(diethylene glycol methyl ether methacrylate) (PEGM) and poly(2,2,2-trifluoroethyl acrylate) (PTFEA) from bacterial cellulose (BC), denoted as BC-g-P(EGM-co-TFEA)). The rigid BC skeleton can significantly enhance the mechanical strength to depress Li dendrite growth. Furthermore, flexible P(EGM-co-TFEA) side chains are able to homogenize lithium-ion flux, inducing the generation of LiF, boost ion conductivity, and maintain good electrode interface contact. As a result, Li/Li symmetric cells with a BC-g-P(EGM-co-TFEA)-protective film enable long-term (1500 h) reversible lithium plating/stripping at a high current density of 10 mA cm–2, while the Li@BC-g-P(EGM-co-TFEA)/LiFePO4 cell maintains a small capacity decay per cycle of 4% during 500 cycles at 3 C. This work could provide an innovative strategy to develop superior artificial SEI films for inhibiting Li dendrite growth on the Li metal anode.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Yue Lei,Xin Xu,Junying Yin,Jianping Xu,Kang Xi,Lai Wei,Haihua Wu,Sen Jiang,Yunfang Gao
Commercial Li-ion batteries use LiPF6-based carbonate electrolytes extensively, but there are many challenges associated with them, like dendritic Li growth and electrolyte decomposition, while supporting the aggressive chemical and electrochemical reactivity of lithium metal batteries (LMBs). This work proposes 1,1,1,3,3,3-hexafluoroisopropyl methacrylate (HFM) as a multifunctional electrolyte additive, constructing protective solid-/cathode-electrolyte interphases (SEI/CEI) on the surfaces for both lithium metal anode (LMA) and Ni-rich cathode to solve these challenges simultaneously. The highly fluorinated group (−CF3) of the HFM molecule contributes to the construction of SEI/CEI films rich in LiF that offer excellent electronic insulation, high mechanical strength, and surface energy. Accordingly, the HFM-derived LiF-rich interphases can minimize the electrolyte–electrode parasitic reactions and promote uniform Li deposition. Also, the problems of LiNi0.8Co0.1Mn0.1O2 particles’ inner microcrack evolution and the growth of dendritic Li are adequately addressed. Consequently, the HFM additive enables a Li/LiNi0.8Co0.1Mn0.1O2 cell with higher capacity retention after 200 cycles at 1 C than the cell with no additive (74.7 vs 52.8%), as well as a better rate performance, especially at 9 C. Furthermore, at 0.5/0.5 mAh cm–2, the Li/Li symmetrical battery displays supersteadfast cyclic performance beyond 500 h when HFM is present. For high-performance LMBs, the HFM additive offers a straightforward, cost-effective route.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Mengli Tao,Guangyuan Du,Wenwu Zou,Jiaqi Cao,Wei Li,Guangli Zheng,Zhenxing Liang,Zhiming Cui,Li Du,Huiyu Song
The performance of thin lithium metal anodes is affected due to issues that weaken the electrode-electrolyte interphase. In this work, a coating layer serving as a Li + traffic controller based on hexadecyl trimethyl ammonium bis(trifluoromethanesulphonyl)imide ([CTA][TFSI]) and poly (vinylidene difluoride co-hexafluoropropylene) (P(VDF-HFP)) is used to stabilize the thin lithium metal interface. The CTA + ions in the coating layer can effectively regulate the distribution of Li + concentration to promote uniform deposition of lithium. The anion of [CTA][TFSI] can optimize solid electrolyte interphase (SEI) with inorganic-rich components, which improve the ionic conductivity and reaction kinetics. Furthermore, the flexible polymer skeleton can fortify the fragile SEI, facilitating the consistent operation of the battery. Due to these improvements, a thin Li metal anode (4 mAh cm −2 ) with a coating layer in a Li||Li symmetric cell demonstrates a lifespan of 600 h at 1 mA cm −2 and 1 mAh cm −2 . Notably, full cells with an ultra-low negative electrode/positive electrode = 1 (N/P = 1) demonstrate a stable performance over 200 cycles and 90 cycles at 0.5C and 1C (1C = 170 mA g −1 ), respectively.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-10
·
IF 16.6
Jin Chengbin,Huang Yiyu,Li Lanhang,Wei Guoying,Li Hongyan,Shang Qiyao,Ju Zhijin,Lu Gongxun,Zheng Jiale,Sheng Ouwei,Tao Xinyong
Reactive negative electrodes like lithium (Li) suffer serious chemical and electrochemical corrosion by electrolytes during battery storage and operation, resulting in rapidly deteriorated cyclability and short lifespans of batteries. Li corrosion supposedly relates to the features of solid-electrolyte-interphase (SEI). Herein, we quantitatively monitor the Li corrosion and SEI progression (e.g., dissolution, reformation) in typical electrolytes through devised electrochemical tools and cryo-electron microscopy. The continuous Li corrosion is validated to be positively correlated with SEI dissolution. More importantly, an anti-corrosion and interface-stabilizing artificial passivation layer comprising low-solubility polymer and metal fluoride is designed. Prolonged operations of Li symmetric cells and Li | |LiFePO 4 cells with reduced Li corrosion by ~74% are achieved (0.66 versus 2.5 μAh h −1 ). The success can further be extended to ampere-hour-scale pouch cells. This work uncovers the SEI dissolution and its correlation with Li corrosion, enabling the durable operation of Li metal batteries by reducing the Li loss.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Chaoqun Niu,Mingke Zhang,Guangping Chen,Bokai Cao,Jiwei Shi,Jie Du,Yong Chen
Polyacrylate polymer is a promising polymer matrix for gel polymer electrolyte (GPE) in lithium-ion batteries . Herein, in-situ polymerized poly(ethylene glycol phenyl etheracrylate) (PEGPEA) based GPE combined with 1 M LiPF6 in ethylene carbonate/dimethyl carbonate/ethyl methyl carbonate (EC/DMC/EMC, 1:1:1 in volume) solvents was introduced. The maximum recoverable strain of the in-situ polymerized PEGPEA-GPE was up to 99%. The outstanding interfacial compatibility between PEGPEA-GPE and the lithium electrode was also obtained. Surprisingly, lithium dendrite was effectively suppressed in charge-discharge cycling because of polymer-enhanced solid electrolyte interphase (SEI) and excellent contact interface. Furthermore, the PEGPEA-GPE exhibited wide electrochemical stability window up to 4.9 V versus Li + /Li, and achieved an ionic conductivity of 3.35 × 10 −3 S cm −1 at 25 °C. When used as electrolyte, the Li[Ni 0.5 Co 0.2 Mn 0.3 ]O 2 /PEGPEA-GPE/Li batteries showed high discharge capacity retention rate of 97.5% after 70 charge-discharge cycles and considerable discharge rate capability, i.e., 155 mAh g −1 0.2C, 142 mAh g −1 0.5C, 120 mAh g −1 1C, 60 mAh g −1 2C. These results demonstrate that this highly elastic in-situ polymerized PEGPEA-GPE is a potential electrolyte system for high-performance polymer electrolyte lithium-ion batteries and has excellent application prospects in wearable and flexible batteries.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
NEW CARBON MATERIALS
·
2023
·
IF 5.7
Xian-lan Ke,Yu-heng Lu,Jin-lun Wu,Ding-cai Wu
We report the fabrication of vulcanized cross-linked polystyrene grafted on carbon nanotubes (CNTs) for use as an advanced three-dimensional Li host. First, polystyrene was grafted from Br-modified CNTs to form brush-like structure by surface-initiated atom-transfer radical polymerization. Polystyrene grafted on carbon nanotubes was then cross-linked using a Friedel-Crafts reaction and finally vulcanized with sulfur. Vulcanized cross-linked polystyrene grafted on carbon nanotubes was used as a support for the Li metal, and its macro-, meso- and microporous structure increased Li ion transport, buffered the volume changes of the Li anode, and provided a high specific surface area to reduce local current density, which assisted rapid and uniform Li plating/stripping. At the same time, the homogenously distributed sulfur in the support reacted with Li to produce a Li 2 S-containing SEI layer, while the CNTs provided conductive pathways for the rapid transmission of electrons. As a result, a Li|Li symmetric cell using this anode material and a Cu current collector had a stable cycling performance of more than 500 h at a current density of 1 mA cm −2 . When LiFePO 4 was used as the cathode, a full cell had a high discharge capacity of 101 mAh g −1 with a capacity retention of 77% after 600 cycles at 1 C.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·Vol. 35
·期 38
·2503713
·
IF 19
Caiyan Shen,Dichang Guan,Wenchao Liu,Yanbing Cao,Zhongdong Peng,Yu Ren,Litao Kang,Jinhao Meng,Zhichen Xue,Ke Du
The development of fluorine-free electrolytes offers a promising route for more environmentally sustainable lithium-ion batteries (LIBs). However, the low solubility of fluorine-free lithium salts in conventional carbonate solvents limits this progress. Additionally, while strongly coordinating solvents enhance salt dissolution, their use can lead to co-intercalation in graphite, complicating electrolyte design. Herein, lithium bis(oxalate)borate (LiBOB) is chosen as lithium salt, and a synergistic electrolyte design strategy is employed, combining a strongly coordinating solvent (tris(2-methylpropyl) phosphine oxide, TMP) and weakly coordinating solvent (dimethyl carbonate, DMC). This approach enables the use of fluorine-free lithium salts while ensuring compatibility with graphite by modulating the primary coordination shell. Furthermore, this solvation structure enables the formation of an inorganic-dominated cathode electrolyte interphase (CEI) on the LiMn 2 O 4 (LMO) and a solid electrolyte interphase (SEI) on the graphite, improving lithium-ion conductivity and overall electrochemical performance. Additionally, compared to lithium hexafluorophosphate (LiPF 6 ), fluorine-free lithium salt minimized the formation of HF by-products, suppressing transition metals (TMs) dissolution. As a result, 1 Ah LMO||graphite pouch cell with fluorine-free electrolyte retains 92.8% of its capacity after 200 cycles, demonstrating excellent cycling stability and delivering high-rate capacity of 0.8486 Ah at 2 C, compared to 84.8% retention and 0.652 Ah with the conventional electrolyte.
研究领域:
电化学
·
能源材料
·
电池技术
·
可持续化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yongrui Luo,Yinnan Qian,Minghui Cai,Pengtao Zhang,Jixiao Li,Zhaoyan Luo,Jiangtao Hu,Yongliang Li,Qianling Zhang,Xiangzhong Ren
Plastic-crystal-embedded elastomer electrolytes (PCEEs), produced through polymerization-induced phase separation (PIPS), are gaining popularity as solid polymer electrolytes (SPEs). However, it remains to be investigated whether all monomer molecules can achieve polymerization-induced phase separation and the corresponding differences in lithium metal battery performance. Herein, we prepared PCEEs with different functional groups ( OH, CN, F) through in situ polymerization. Research findings show that PCEE containing – CN or – F achieves the separation of the plastic crystalline phase and succinonitrile (SN) phase, whereas PCEE containing OH cannot due to hydrogen bonding with the SN phase. Notably, the PCEE synthesized with the F monomer (FBA-PCEE) exhibited exceptional interfacial stability with lithium metal anodes and lithium iron phosphate (LFP) cathodes, due to its unique coordination mechanism with lithium ions. The FBA-PCEE demonstrated a high ionic conductivity (2.02 × 10 −3 S cm −1 ) and lithium-ion migration number ( t Li + = 0.75). Moreover, lithium symmetric cells incorporating FBA-PCEE demonstrated stable cycling performance for more than 1000 h at a current density of 0.1 mA cm −2 , resulting in the development of a solid electrolyte interphase (SEI) rich in LiF, Li 3 N, and Li 2 CO 3 over time. Additionally, incorporating FBA-PCEE facilitated the stable cycling of LPF over 1000 cycles at 0.5C, maintaining a capacity retention of 77.38 % after 500 cycles. When coupled with high-voltage Nickel Cobalt Manganese Oxide (NCM-622) cathodes and lithium metal anodes, a discharge capacity of 119.70 mAh g −1 at 0.1C was sustained after 100 cycles, exhibiting a capacity retention of 78.95 %. This study elucidates the critical role of monomer design in achieving PIPS, offering valuable insights into developing high-performance polymer composite electrolytes for advanced lithium metal batteries.
研究领域:
材料科学
·
电化学
·
电池技术
·
高分子化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 11
·期 4
·1966-1977
·
IF 14.511
Zhiheng Ren,Jixiao Li,Minghui Cai,Ruonan Yin,Jianneng Liang,Qianling Zhang,Chuanxin He,Xiantao Jiang,Xiangzhong Ren
Polymer electrolytes (PEs) synthesized from an in situ polymerization strategy are considered as promising candidates to improve interfacial compatibility. However, most in situ formed PEs still suffer from problems such as low lithium-ion transference number (tLi+) and insufficient ionic conductivity at room temperature (RT). Herein, a series of copolymer electrolytes (CPEs) consisting of 1,3-dioxolane (DOL) and 1,3,5-trioxane (TXE) monomers are synthesized. Due to the additive of succinonitrile (SN), and the promoted dissociation of lithium salt, the obtained polymer electrolyte (SN-CPE) exhibits an excellent ionic conductivity (4.06 × 10−4 S cm−1) and a high lithium-ion transference number (tLi+ = 0.881) at RT, as well as a high voltage oxidation window of 5.1 V. Thanks to the in situ formed intimate contacted electrode/electrolyte interface, the symmetric Li/Li cell can achieve long-term cycling stability over 1500 h without a short circuit. A LiF-rich organic–inorganic composite layer is formed on both the solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI) as demonstrated by XPS, TEM, and SEM analyses. Thereafter, the LiFePO4/Li cell has a high capacity retention of 84.1% after 900 cycles at RT, and it can still work effectively at high temperatures (e.g. 80 °C). Furthermore, SN-CPE exhibits excellent electrochemical performance and safety in the LiCoO2/Li cell and LiFePO4/graphite pouch cell, which again supports the promising application of SN-CPE.
研究领域:
材料科学
·
电化学
·
能源存储
·
电池技术
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Minghui Kong,Wenlong Wang,Jiaqiang Li,Qiang Yang,Runru Liu,Qi Liu,Daobin Mu,Li Li,Renjie Chen,Shuo Yang,Bin Wang,Feng Wu
This research explores the structural and interfacial regulation mechanisms of multi-element synergistic electrolytes for high voltage LiNi x Co y Mn 1-x-y O 2 (NCM) lithium ion batteries through a combined simulation-experiment approach. Theoretical calculations revealed that difluoroxalate borate ion (DFOB − ) exhibit a pronounced negative electrostatic potential distribution, with a binding energy to Li + (-110.26 kJ/mol) higher than conventional carbonate solvents (e.g., DMC, FEC), thus dominating the formation of anion-enriched solvation sheaths and significantly reducing Li + desolvation energy barriers (<30 kJ/mol). Raman spectroscopy and molecular dynamics simulations confirmed that LiDFOB introduction facilitates the transition of solvation structures from solvent-separated ion pairs (SSIPs) to contact ion pairs (CIPs) and aggregates (AGGs), with CIPs/AGGs proportion increasing from 29 % to 39 %, effectively suppressing LiPF 6 hydrolysis and mitigating electrode structural damage caused by solvent co-intercalation. Electrochemical tests demonstrated that the optimized 0.5 PB modified electrolyte(0.5 M lithium hexafluorophosphate+0.5 M lithium difluoro(oxalato)borate dissolved in a mixed solvent of dimethyl carbonate: fluoroethylene carbonate: propyl p-toluene sulfonate in a ratio of 3:1:1) enabled NCM811||Li half-cells to achieve 88 % capacity retention after 100 cycles at 4.5 V high voltage (versus 58 % for control group), along with stable lithium metal anode cycling for 500 h at 1 mA·cm −2 . Interface analysis revealed that DFOB⁻ and PPTs preferentially undergo redox reactions to form inorganic-rich cathode electrolyte interphase (CEI) films containing borides (LiₓBOyFz) and sulfonates (ROSO₂Li). On the anode side, synergistic effects of DFOB⁻, Propyl p-toluene sulfonate (PPTs) and FEC generate LiF/sulfur/boride-enriched composite solid electrolyte interface (SEI) layers, effectively suppressing transition metal dissolution and graphite structural degradation. This work provides a novel paradigm of "anion coordination-solvation structure-interface functionalization" for high-voltage lithium-ion batteries."
研究领域:
电化学
·
能源材料
·
锂离子电池
·
电池界面工程
·
计算材料科学
✓ 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）