Advanced Energy Materials
·
2022
·Vol. 12
·期 44
·2202253
·
IF 29.698
Zhenjie Cheng,Longfei Guo,Qingyu Dong,Chunting Wang,Qian Yao,Xin Gu,Jian Yang,Yitai Qian
Dual-ion batteries have shown promising prospect in energy storage, owing to their low material costs, high power capability, and environmental friendliness. However, graphite as the cathode always suffers from structural damage and electrode/electrolyte interface instability, which greatly deteriorate their electrochemical performance. Here, tris(trimethyl-silyl) phosphite (TMSP) is added as an electrolyte additive to improve the electrochemical performance. TMSP not only scavenges the deleterious species generated by electrolytes, but also produces a thin and uniform cathode–electrolyte interphase layer on graphite. Hence, the electrochemical performance is greatly promoted. In graphite||graphite, the capacity retention is ≈96.8% at 30 °C or 92.5% after 3000 cycles in the presence of TMSP, much better than those without TMSP (62% at 30 °C or 27% after 200 cycles).
研究领域:
电化学
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能源材料
·
储能技术
·
先进电池
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界面化学
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
·
2025
·
IF 14.9
Linjun Zhong,Ziqiang Fan,Zhe Wang,Xinyue Wu,Jingan Liu,Junjun Liu,Junyang Zheng,Qing Chen,Lidan Xing,Jianhui Li,Yu Ying,Ronghua Zeng
Almost all commercial lithium-ion batteries (LIBs) with LiCoO 2 (LCO) as cathode material are cycled from 3.0 to 4.2 V and their actual specific capacity just ranges from 140 to 160 mA h g −1 , which is much lower than the theoretical specific capacity of LCO of 274 mA h g −1 . To further improve the actual specific capacity of LCO, elevating the upper limit of its working voltage is necessary. However, as the upper limit of its working voltage is elevated to 4.5 V or higher, the LCO crystal will undergo severe irreversible phase transition, and the oxidization decomposition of electrolyte on the cathode’s surface will exacerbate, which will severely reduce the cycling lifespan of batteries, hindering the actual application of high voltage LCO. In this work, we find that 3,5-difluorophenylboronic acid pinacol ester (35-DAPE) is an effective cathode electrolyte interphase (CEI)-forming additive, which can form a robust and stable CEI layer rich in fluorophenyl-groups and B–F/B–O bonds on the surface of LCO cathode, inhibiting the dissolution of cobalt ions and maintain the structural stability of LCO crystal over cycles. The graphite||LCO pouch cells in a voltage range of 3.0–4.5 V with 35-DAPE display a capacity retention rate of 91.1% after 150 cycles at room temperature, compared to that of 2.4% in baseline electrolyte. Besides, rate performance at room temperature and discharging performance at low temperatures of graphite||LCO pouch cells can also be observed with an improvement after the introduction of 35-DAPE. In addition, this work has explained the decomposition mechanism of 35-DAPE and how its products improve the electrochemical performance of graphite||LCO pouch cells in detail, which not only advances the actual application of fluorophenylboronic acid pinacol ester additive in high voltage LIBs but also provides valuable insights for the design of functional electrolyte additives.
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DOI
高影响因子
Energy Storage Materials
·
2024
·
IF 18.9
Zhengzheng Ru,Meilan Peng,Said Amzil,Shengyao Luo,Tonghui Xu,Ye Yue,Mengqi Wu,Ya-Jun Cheng,Yonggao Xia
Lithium-ion batteries with high-nickel cathode materials are promising candidates for achieving significantly higher energy densities. However, when Ni-rich subjected to higher charging cutoff voltages accelerates both electrolyte decomposition and structural degradation, leading to compromised cycling stability and reduced lifespan. In this study, we have developed a dual-additive strategy using lithium difluoro bisoxalate phosphate (LiDFBOP), and 1,3-divinyl-1,1,3,3-tetramethyldisilazane (DTDS) to address these challenges and improve the battery's performance. Theoretical calculations and experimental results indicate that the LiDFBOP regulates Li⁺ solvation for robust CEI formation, while DTDS scavenges impurities and promotes the formation of an inorganic/organic interphase. The synergistic effect of these additives combination allows Li||NCM811 coin cell to retain a capacity retention 87.9 % at 4.6 V and Graphite||NCM811full cell achieved 90.5 % capacity retention at 4.5 V. Moreover, the 1Ah pouch full cells exhibit excellent cycling stability, with a capacity retention of 91.4 % after 610 cycles at a constant current of 500 mA and voltage of 4.5 V. This work offers guidance on designing multifunctional additives to achieve synergistic electrolyte engineering for high-energy lithium-ion batteries.
研究领域:
电化学
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材料科学
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能源存储
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电池技术
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界面化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2025
·
IF 4.1
Zhicheng Dai,Shiyu Cao,Wenfeng Shi,Bokang Liu,Guanchao Yin,Fei Chen
Increasing the voltage of lithium batteries represents the most direct and effective strategy for enhancing battery capacity. However, excessively high charging voltages can result in the degradation of battery interfacial contacts and the dissolution of transition metals in the cathode, thereby limiting the cycling performance of the battery. This paper employs a fluorosulfonic acid salt electrolyte as a sacrificial agent to in situ construct a stable CEI (Cathode Electrolyte Interface) and SEI (Solid Electrolyte Interface). The resulting membrane is characterized by a uniform distribution of LiF and LiSO x , which exhibit high lithium-ion conductivity and mitigate dissolution of active materials under high voltage. This membrane effectively restricts further electrolyte consumption, allowing the remaining electrolyte to wet the interface and reduce interfacial impedance adequately. Moreover, the CEI can suppress the dissolution of transition metals from the cathode and prevent them from shuttling to the anode side. When implemented in lithium batteries, the use of the sacrificial agent enables the NCM523/Li battery (with an initial discharge capacity of 105 mAh/g) to achieve a high capacity retention of 85.7 % after 800 cycles at a 1 C rate and 30 °C.
研究领域:
电化学
·
材料科学
·
能源存储
·
电池技术
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界面化学
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锂离子电池
✓ 已验证
产品关联
DOI
高影响因子
Science Bulletin
·
2022
·
IF 20.577
Fangyuan Cheng,Xiaoyu Zhang,Peng Wei,Shixiong Sun,Yue Xu,Qing Li,Chun Fang,Jiantao Han,Yunhui Huang
The LiNi 0.8 Co 0.1 Mn 0.1 O 2 (Ni-rich NCM) cathode materials suffer from electrochemical performance degradation upon cycling due to detrimental cathode interface reactions and irreversible surface phase transition when operating at a high voltage (≥4.5 V). Herein, a traditional carbonate electrolyte with lithium difluoro(oxalato)borate (LiDFOB) and tris(trimethylsilyl)phosphate (TMSP) as dual additives that can preferentially oxidize and decompose to form a stable F, B and Si-rich cathode-electrolyte interphase (CEI) that effectively inhibits continual electrolyte decomposition, transition metal dissolves, surface phase transition and gas generation. In addition, TMSP also removes trace H 2 O/HF in the electrolyte to increase the electrolyte stability. Owing to the synergistic effect of LiDFOB and TMSP, the Li/LiNi 0.8 Co 0.1 Mn 0.1 O 2 half cells exhibit the capacity retention 76.3% after 500 cycles at a super high voltage of 4.7 V, the graphite/LiNi 0.8 Co 0.1 Mn 0.1 O 2 full cells exhibit high capacity retention of 82.8% after 500 cycles at 4.5 V, and Li/LiNi 0.8 Co 0.1 Mn 0.1 O 2 pouch cells exhibit high capacity retention 94% after 200 cycles at 4.5 V. This work is expected to provide an effective electrolyte optimizing strategy compatible with high energy density lithium-ion battery manufacturing systems.
研究领域:
电化学
·
材料科学
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能源存储
·
锂离子电池
·
界面化学
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
·
2024
·
IF 14
Yilin Zhang,Yuqing Chen,Qiu He,Jinlong Ke,Wei Wang,Jian-Fang Wu,Peng Gao,Yanhua Li,Jilei Liu
The Li metal battery with ultrahigh-nickel cathode (LiNi x M 1− x O 2 , M = Mn, Co, and x ≥ 0.9) under high-voltage is regarded as one of the most promising approaches to fulfill the ambitious target of 400 Wh/kg. However, the practical application is impeded by the instability of electrode/electrolyte interface and Ni-rich cathode itself. Herein we proposed an electron-defect electrolyte additive trimethyl borate (TMB) which is paired with the commercial carbonate electrolyte to construct highly conductive fluorine- and boron-rich cathode electrolyte interface (CEI) on LiNi 0.9 Co 0.05 Mn 0.05 O 2 (NCM90) surface and solid electrolyte interphase (SEI) on lithium metal surface. The modified CEI effectively mitigates the structural transformation from layered to disordered rock-salt phase, and consequently alleviate the dissolution of transition metal ions (TMs) and its “cross-talk” effect, while the enhanced SEI enables stable lithium plating/striping and thus demonstrated good compatibility between electrolyte and lithium metal anode. As a result, the common electrolyte with 1 wt% TMB enables 4.7 V NCM90/Li cell cycle stably over 100 cycles with 70% capacity retention. This work highlights the significance of the electron-defect boron compounds for designing desirable interfacial chemistries to achieve high performance NCM90/Li battery under high voltage operation.
研究领域:
电化学
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材料科学
·
能源存储
·
锂电池技术
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界面化学
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固态电解质界面
·
功能材料
✓ 已验证
DOI
高影响因子
Carbon Energy
·
2025
·
IF 24.2
Chang Guo,Xin-Yu Fan,Mengting Liu,Shao-Wen Xu,Guang-Xu Wei,Zhen-Bang Chen,Zhao-Kun Guan,Yao Xiao,Hanshen Xin,Peng-Fei Wang
Although sodium-ion batteries (SIBs) are competitive for large-scale electrical energy storage, the high-voltage instability of the cathode–electrolyte interphase (CEI) formed on the cathode surface results in the dissolution of the transition metal (TM) and the sluggish interfacial electrochemical reaction kinetics, which deteriorates both the energy density and the cycle life of the SIBs. Herein, we propose a surface modification strategy to reconstruct the interphase of P2-type Na 0.7 Li 0.03 Mg 0.03 Ni 0.27 Mn 0.6 Ti 0.07 O 2 (LM′NMT) cathode with amorphous SiO 2 (denote as SiO 2 @LM′NMT) by a wet chemical method. This approach facilitates the reconfiguration of a more stable, inorganic-rich CEI due to enhanced adsorption catalysis of an amorphous coating with ample defects, resulting in improved Na + transport kinetics and inhibition of subsequent side reactions, TM dissolution, and structural degradation. As a result, the modified SiO 2 @LM′NMT-5 cathode exhibits an impressive capacity of 131.6 mAh g −1 at 0.1 C and maintains exceptional cycling stability, with 91.7% capacity retention after 150 cycles at 1 C within the voltage window of 2.2 to 4.4 V. This study grasps insights into optimizing the CEI to push forward practical application of SIBs under high voltages.
研究领域:
材料科学
·
电化学
·
能源存储
·
纳米材料
·
界面化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Xuelian Liu,Quan Zong,Keyi Chen,Chaofeng Liu,Yongchun Ye,Qiaoling Kang,Jingji Zhang,Qilong Zhang,Chenbin Jin,Guozhong Cao
Pre-intercalation has emerged as a highly effective strategy to enhance structural integrity and ion transport kinetics in cathodes for aqueous Zn-ion batteries. Here, we report a zinc-ion pre-intercalated hydrate vanadium oxide cathode, in which the initial insertion of Zn 2+ induces a significant expansion of the interplanar spacing, followed by contraction at higher Zn 2+ concentrations owing to strong electrostatic interactions with the V O framework. Such competing expansion and contraction of interplanar spacing enhances the overall electrochemical properties. In addition, the pre-intercalated Zn 2+ facilitates the in situ formation of a Zn 3 (OH) 2 V 2 O 7 ·2H 2 O cathode-electrolyte interphase (CEI) layer, which not only suppresses vanadium dissolution but also regulates the desolvation of hydrated Zn 2+ , thus further enhancing the structural integrity and interfacial kinetics. Benefiting from these merits, the Zn 2+ pre-intercalated hydrate vanadium pentoxide (denoted as 2Zn-VOH) cathode delivers a high capacity of 395 mA h g −1 at 0.1 A g −1 , exhibits excellent cycling stability at both low and high current densities, and retains outstanding performance under low-temperature conditions (295 mAh g −1 at 0.1 A g −1 and − 10 °C, with 83.8 % capacity retention after 1000 cycles at 0.2 A g −1 ).
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Hong Tan,Pan Wang,Guocai Yuan,Huan Yang,Jiang Ye,Kai Lu,Gang Chen,Biyou Peng,Qinyong Zhang
The advancement of aqueous zinc-ion batteries (AZIBs) is impeded by challenges encompassing cathodic and anodic aspects, such as limited capacity and dendrite formation, constraining their broader utilization. Herein, pyrrole, an economically viable and readily accessible compound, is proposed as a versatile electrolyte additive to address these challenges. Experiments and DFT calculations reveal that pyrrole and its derivatives preferentially adsorb onto zinc foil, facilitating the formation of a pyrrole-based solid electrolyte interphase (SEI), which effectively guides uniform Zn 2+ deposition through strong attraction force and suppresses hydrogen evolution reactions and parasitic reactions. On the cathode side, the additive promotes the formation of a durable cathode electrolyte interphase (CEI) enriched with poly-pyrrole (Ppy) analogues. Such layer significantly contributes to extra capacity of both polyaniline (PANI) and MnO 2 cathodes by leveraging the electrochemical reactivity of Ppy towards Zn 2+ and improves their cyclic stability. Consequently, a dendrite-free Zn anode is realized with an extended cyclic lifespan surpassing 6000 h in Zn//Zn cell, coupled with an average Coulombic efficiency of 99.7 % in Cu//Zn cell. Moreover, the PANI//Zn and MnO 2 //Zn full cells demonstrate enhanced capacities along with improved cycling stability. This work provides a new additive strategy towards concurrent stabilization of cathode and Zn anode in AZIBs.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Energy Materials
·
2025
·Vol. 15
·期 33
·2502363
·
IF 26
Xinyou He,Haozhe Qin,Junxiang Liu,Jiaqi Wang,Zhiming Xiao,Lei Ming,Tongchao Liu,Khalil Amine,Xing Ou
Gel polymers are regarded as a promising candidate electrolyte for lithium-metal quasi-solid-state batteries, primarily due to their high ionic conductivity and solid-liquid synergistic properties. However, challenges such as interfacial side reactions, limitations in Li + transport caused by interfacial issues, and leaching of transition metals from the cathode have yet to be effectively solved. Herein, a novel gel electrolyte modulation strategy based on electrostatic filler assembly is proposed to address the issues of ineffective capacity utilization and inadequate cycling stability of high-energy-density cathode materials in solid-state lithium-ion batteries. It constructs a 3D interpenetrating charge-bridge network that effectively tackles the phase-separation challenge between fillers and electrolytes at the molecular level. Meanwhile, the molecular interlocking structure effectively inhibits the electrolyte erosion. More critically, it optimizes and stabilizes the cathode-electrolyte interface film, which facilitates the conduction of Li⁺-ions through a size-sieving mechanism. Consequently, this strategy enables effective adaptation across diverse high-energy-density cathode materials with satisfactory capacity performance (170.4 mAh g −1 at 4.5 V/1 C for LiNi 0.6 Co 0.2 Mn 0.2 O 2 and 194.0 mAh g −1 at 4.3 V/1 C for LiNi 0.9 Co 0.08 Mn 0.02 O 2 ). This investigation offers a straightforward and effective reference for addressing the critical challenges of ionic transport and interface stabilization in the design of gel electrolytes.
研究领域:
材料科学
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电化学
·
储能技术
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锂离子电池
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高分子科学
✓ 已验证
产品关联
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
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电化学
·
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
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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）