JOURNAL OF POWER SOURCES
·
2022
·
IF 9.794
Fengwei Bai,Yan Li,Ziyu Chen,Yongchao Zhou,Chengzong Li,Tao Li
High-voltage lithium (Li)-metal batteries with cell-level energy density over 350 Wh kg −1 are promising energy storage systems . However, the aggressive interphase chemistries associated with highly reactive Li-metal anode and high-voltage cathodes impede their practical applications. Herein, we demonstrate the targeted stabilization of solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI) in high-voltage Li-metal batteries by asymmetrically sustained-releasing different additives. An asymmetric sustained-release film loaded with lithium bis-(oxalate)borate (LiBOB) and LiNO 3 on each side is investigated as a proof-of-concept. The sustained-releasing of LiBOB and LiNO 3 can maintain a localized concentration at the high-voltage cathode and Li-metal anode fronts respectively, thus forming a stable B-containing CEI and N-containing SEI. As such, issues like dendrites growth, parasitic side reactions and transition metals dissolution under high-voltage are addressed simultaneously. Based on this strategy, the 30 μm Li|LiNi 0.5 Co 0.2 Mn 0.3 O 2 (4.1 mAh cm −2 ) batteries deliver a capacity retention of 80% after 173 cycles under a cut-off voltage of 4.5 V.
研究领域:
储能系统
·
电池技术
·
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
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
·
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
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
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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
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能源材料
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电池技术
·
可持续化学
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材料科学
✓ 已验证
产品关联
DOI
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）