MOLECULES
·
2022
·Vol. 27
·期 22
·7827
·
IF 4.927
Yunhao Zhao,Yueyue Wang,Rui Liang,Guobin Zhu,Weixing Xiong,Honghe Zheng
The overall electrochemical performance of natural graphite is intimately associated with the solid electrolyte interphase (SEI) layer developed on its surface. To suppress the interfacial electrolyte decomposition reactions and the high irreversible capacity loss relating to the SEI formation on a natural graphite (NG) surface, we propose a new design of the artificial SEI by the functional molecular cross-linking framework layer, which was synthesized by grafting acrylic acid (AA) and N,N′−methylenebisacrylamide (MBAA) via an in situ polymerization reaction. The functional polymeric framework constructs a robust covalent bonding onto the NG surface with —COOH and facilitates Li+conduction owing to the effect of the —CONH group, contributing to forming an SEI layer of excellent stability, flexibility, and compactness. From all the benefits, the initial coulombic efficiency, rate performance, and cycling performance of the graphite anode are remarkably improved. In addition, the full cell using the LiNi0.5Co0.2Mn0.3O2cathode against the modified NG anode exhibits much-prolonged cycle life with a capacity retention of 82.75% after 500 cycles, significantly higher than the cell using the pristine NG anode. The mechanisms relating to the artificial SEI growth on the graphite surface were analyzed. This strategy provides an efficient and feasible approach to the surface optimization for the NG anode in LIBs.Keywords:natural graphite;artificial SEI;in situ polymerization;lithium-ion batteries
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Hao Wu,Wenfang Feng,Michel Armand,Zhibin Zhou,Heng Zhang
Carbonyl-based negative electrodes have received considerable interest in the domain of rechargeable lithium batteries, owing to their superior feasibility in structural design, enhanced energy density, and good environmental sustainability. Among which, lithium terephthalate (LiTPA) has been intensively investigated as a negative electrode material in the past years, in light of its relatively stable discharge plateau at low potentials (ca. 1.0 V vs Li/Li+) and high specific capacity (ca. 290 mAh g–1). However, its cell performances are severely limited owing to the poor quality of the solid-electrolyte-interphase (SEI) layer generated therein. Here, we report the utilization of lithium bis(fluorosulfonyl)imide (LiFSI) as an electrolyte salt for forming a Li-ion permeable SEI layer on the LiTPA electrode and subsequently improving the cyclability and rate performance of the LiTPA-based cells. Our results show that, differing from the reference electrolyte containing the lithium hexafluorophosphate (LiPF6) salt, the electrochemical reductions of the FSI– anions occur prior to the lithiation processes of LiTPA electrode, which is capable of building an inorganic-rich SEI layer containing lithium fluoride (LiF) and lithium sulfate (Li2SO4). Consequently, the lithium metal (Li°)||LiTPA cell shows significantly improved cycling performance than the LiPF6-based reference cell. This work provides useful insight into the reductive processes of the FSI– anions on negative electrodes, which could spur the deployment of highly sustainable and high-energy rechargeable lithium batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Next Materials
·
2026
·
IF 4.7
Zhichun Si,Xinhua Zhou,Haofeng Wu,Chunguang Wei,Feiyu Kang
Zinc anodes suffer from dendrite growth and side reactions, limiting Coulombic efficiency (CE) and cycling stability. Constructing a stable solid electrolyte interphase (SEI) is critical, yet the electrolyte structure–SEI relationship remains unclear. Here, we introduce tetraethylene glycol dimethyl ether (TEGDME) into aqueous Zn(OTf) 2 electrolyte. Unlike conventional additives, TEGDME does not enter the primary Zn(H₂O)₆²⁺ solvation shell but alters the secondary solvation shell, disrupting hydrogen bonding and facilitating solvent−separated ion pairs (SSIPs, e.g., Zn 2 + –H 2 O–OTf⁻). This creates an “organic–inorganic hybrid” solvation structure, leading to a gradient hybrid SEI with a ZnF₂−rich outer layer and an inner layer enriched in organic species, ZnS, and ZnCO 3 . This SEI enables dendrite−free Zn deposition and suppresses side reactions. Consequently, the Zn||Cu cell achieves 99.76% CE, the Zn||Zn symmetric cell cycles for 2400 h, and the Zn||VOH full cell retains 80% capacity after 1100 cycles, far outperforming the unmodified electrolyte.
✓ 已验证
产品关联
DOI
高影响因子
Small Methods
·
2025
·Vol. 9
·期 11
·e01148
·
IF 9.1
Wei Wu,Changsheng Song,Jiafeng Ruan,Nanyu Chen,Fei Yan,Fang Fang,Dalin Sun,Jie Zhao,Yun Song
The combination of Na metal with a 3D scaffold has effectively solved the long-standing problems of sodium metal batteries, including dendrite formation and volume change. However, uncontrollable interfacial reaction and morphology degradation caused by the high surface area of the scaffold are still unsolved. Here, a solvent pretreatment strategy is reported to generate a pre-formed solid electrolyte interface (SEI) protected Na exclusively confined in the scaffold. This pre-formed SEI prevents the reactive Na from the direct contact with the electrolyte, thereby mitigating side reactions. Meanwhile, by removing the highly reactive Na nanoparticles, as well as their low ionic conductivity derivatives on the surface, this exclusively confined Na structure enhances the uniformity of Na plating/stripping and the corresponding ion transport kinetics. Benefiting from this pre-formed SEI optimization, a thin and NaF-riched SEI can be further evolved during cycling. Compared to the pristine counterpart, Na 3 V 2 (PO 4 ) 3 coupled with the anode protected by pre-formed SEI exhibits a 14.9% and 18.9% increase in specific capacity at 25 and −30 °C, respectively. The pre-formed SEI strategy solves the prolonged interfacial issues of high surface area Na metal composite anodes, and brings a new perspective to the plating/stripping behaviors.
研究领域:
材料科学
·
电化学
·
能源存储
·
纳米材料
·
电池技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Fan Ding,Shuai Liu,Hao Xu,Zhiang Li,Zhenhua Yan,Hongzhi Cui
Lithium metal is regarded as a highly promising anode material for rechargeable batteries, owing to its exceptional specific capacity and energy density. Solid electrolyte interface (SEI) is a key factor influencing the stability of lithium metal anode. Nonetheless, a notable obstacle persists in the unregulated electrodeposition of lithium and the erratic development of the synthetic solid electrolyte interface (SEI) throughout cycling, leading to premature cell malfunction and safety hazards. This study introduces an artificial SEI for lithium metal characterized by consistent Li-ion conveyance and superior mechanical durability to tackle these pivotal challenges. The addition of Vinylidene carbonate (VC) introduces strong polar groups to the SEI, which alters the electron transfer kinetics and facilitates the cleavage of bis (trifluoromethanesulfonimide) (LiTFSI). Consequently, an LiF-rich SEI is formed, which facilitates rapid Li-ion transport and suppresses lithium dendrite growth. The mechanical strength of artificial SEI can be effectively increased, and the risk of lithium dendrite growth reduced by LLZTO. Lithium symmetric cells modified by this artificial SEI can cycle stably at ultra-high current densities (25 mA cm −2 , 25 mAh cm −2 ) for >14,000 h, representing the most prolonged reported cycling duration for lithium metal batteries under such elevated current densities (25 mA cm −2 ). The full cell with LiFePO 4 (LFP) cathode still exhibits a coulombic efficiency of 99 % after 1000 charge/discharge cycles at 0.5C under low-temperature conditions (−2 °C). The rational design not only provides a new strategy for constructing artificial SEI, but also suggests a new approach for the optimization of other battery systems.
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Yitong Zhang,Xiangfei Xu,Hong Huo,Jianjun Zhou,Lin Li
Poly(acrylic acid) copolymers containing nitrile and hydroxyl groups are synthesized through free radical polymerization and used as binders for silicon anodes. The characteristics of these poly(acrylic acid) copolymers are that they can be further in situ cross-linked through the Ritter reaction. The cross-linked binder (c-PACH-2) can simultaneously address the challenges of mechanical degradation, sluggish kinetics, and interfacial instability in the Si anode. The cross-linked architecture can mitigate volume expansion and prevent particle pulverization via elastic stress dissipation. Concurrently, ionic pathways and hopping sites accelerate Li+ diffusion, enabling superior rate capability. Density functional theory calculations and X-ray photoelectron spectroscopy analyses reveal c-PACH-2’s preferential reduction to form a robust LiF-rich SEI film, reducing parasitic reactions. The c-PACH-2 binder delivers exceptional electrochemical performance, and the c-PACH-2@Si||Li cell has a capacity retention of 67.2% after 100 cycles at 0.2 C. This covalent network design integrates mechanical resilience and ion transport in the binders for the Si anode, offering an effective strategy for developing high-performance batteries.
研究领域:
材料科学
·
电化学
·
储能技术
·
高分子化学
·
电池技术
✓ 已验证
DOI
PubMed
高影响因子
Energy Storage Materials
·
2022
·
IF 20.831
Jingning Lai,Nan Chen,Fengling Zhang,Bohua Li,Yanxin Shang,Liyuan Zhao,Li Li,Feng Wu,Renjie Chen
High energy density lithium-oxygen (Li-O 2 ) batteries require soluble catalysts to accelerate the kinetics of oxygen reduction/evolution reaction (ORR/OER), and require SEI forming additives to protect lithium metal anode from side reaction with solvents, reduced oxygen species and soluble catalysts. In this study, a tri-functional additives 1-methyl, 3-benzyl, 1H imidazolium bromide (IMPBr) is dissolved in the dimethyl sulfoxide (DMSO)-based electrolyte to solve the problems of the slow dynamic process of ORR and OER, and protect the lithium anode by suppressing the dendrite formation in O 2 atmosphere. During discharging, IMP + has a strong binding ability to the intermediate product O 2 − , and Br − is highly associated with Li + , helping drive the solvation mechanism. During charging, Br − mediates the decomposition of battery discharge products and reduces the charge overpotential. Meanwhile, the positively charged IMP + can be attracted to the surface of the anode via electric attraction, in situ forming a stable SEI layer to prevent DMSO, Br 3 – , and Br 2 from attacking the lithium metal and growth of lithium dendrites. The synergy effect of the IMP + and Br – improves the cycle and rate performance of the Li-O 2 battery.
研究领域:
电化学
·
材料科学
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Yu Peng,Jiawei Chen,Gaopan Liu,Yue Yin,Xiaoli Fang,Yonggang Wang,Xiaoli Dong,Yongyao Xia
Lithium metal batteries (LMBs) with Li metal anodes and high-voltage LiCoO 2 (LCO) cathodes offer high energy density but face challenges such as Li dendrite growth and LCO structure degradation, which primarily arises from the electrolyte's inability to form a stable interphase. Herein, a dual-additive optimized carbonate-based electrolyte is developed, incorporating tetraethylammonium nitrate (TEANO 3 ) and lithium difluorobis(oxalato) phosphate (LiDFBOP) as regulators. LiDFBOP enhances interfacial stability and compactness, while TEANO 3 facilitates Li + transport and suppresses excessive decomposition of LiDFBOP. The synergistic effect of TEANO 3 and LiDFBOP establishes robust, high ion-conductive solid electrolyte interphase (SEI) and cathode–electrolyte interphase (CEI) enriched with P- and N-containing inorganic compounds (including LiN x O y and P-O/P-F species), enabling dense Li deposition and stable cycling of LCO under a high cut-off voltage of 4.5 V. The optimized electrolyte enables Li||LCO full cells with a high capacity retention of 84% even with high-mass-loading LCO cathode (3.5 mAh cm −2 ) and limited Li (N/P = 2). This work demonstrates a straightforward electrolyte design strategy for optimizing SEI and CEI, advancing the practical deployment of LMBs.
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 POWER SOURCES
·
2020
·
IF 8.247
Shiyou Li,Li Yang,Peng Wang,Zhaojuan Li,Wenbo Li,Haining Liu,Xiaoling Cui
A blank comparison group of lithium salt-free electrolyte system, replacing the lithium salt of electrolyte with a redox shuttle agent, is constructed to give targeted research on the single role of lithium bis(oxalate)borate (LiBOB) salt, especially of bis(oxalate)borate anions (BOB − ) in the film-forming process. By combining and comparing all available studies, such as attenuated total reflectance (IR-ATR), X-Ray photoelectron diffraction spectrum (XPS), electrochemical impedance spectrum (EIS), scanning electron microscopy (SEM) tests and quantum chemical calculation , the formation mechanism of the solid electrolyte interphase (SEI) film is proposed. Results reveal that the prior reduction of BOB − anions can postpone the reduction potential and hinder the decomposition rate of carbonate solvents, but promote the formation of a dense, conductive and effective SEI film. This work provides a novel way to investigate the film-forming mechanism and has guiding significance for revealing the effect of other kinds of lithium salts on the surface film formation.
研究领域:
电化学
·
材料科学
✓ 已验证
DOI
高影响因子
Batteries & Supercaps
·
2023
·Vol. 6
·期 7
·e202300144
·
IF 5.7
Qiongjie Ke,Qingshuai Xu,Xuejun Lai,Minghui Li,Jianhui Li,Keyou Yan,Yongcai Qiu
Graphical Better solubility helps : DMF was used as solubilizer to address the dissolution obstacle of LiNO 3 in carbonate electrolyte. The as-formed inorganic-rich SEI possesses high ionic diffusivity, low chemical activity and high mechanical strength. The designed carbonate electrolyte exhibits enhancing cycling performance over 700 h. Carbonate electrolytes have been extensively used as commercial electrolytes in lithium-ion batteries (LIBs) because of its high oxidative stability. However, the organic-inorganic solid electrolyte interphase (SEI) formed on the lithium (Li) metal surface is too fragile to endure huge volume fluctuation during Li plating/stripping cycles in carbonate electrolytes. Herein, a chemically stable inorganic-rich SEI was constructed on Li metal anodes by dissolving 5.5 M LiNO 3 in N,N-dimethylformamide (DMF) into carbonate electrolytes as an additive. The Li + solvation structure coordinated with NO 3 − and DMF molecules favors the formation of Li x N y , LiN x O y , and LiF in the SEI film, which have been proved to increase the interfacial energy and improve the ionic diffusion as well as the mechanical strength of the SEI. Therefore, the designed carbonate electrolyte enhances the stable cycling of Li symmetric cells up to 700 h, with a high Coulombic efficiency (CE) of 99.0 % by Aurbach CE test. When paired with LiFePO 4 cathode, the coin cells achieve an outstanding average CE of 99.5 % and 86.5 % retention of initial capacity after 300 cycles.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
IONICS
·
2024
·
IF 2.4
Liu Liyang,Zhao Xufan,Qi Jiaxing,Abdussalam Abubakar,Zhang Wei,Wang Hongyu,Xu Guobao
Since the concept of hybrid Li/Na-ion batteries (HLNIBs) was proposed, many cathode materials with excellent performance and low cost have been studied. However, in HLNIBs, mixed cationic electrolyte is formed as Na + is extracted from the cathode, resulting in relatively complicated and unstable electrochemical performance, especially for the half-cell test with lithium metal as the anode. It is necessary to consider the tolerance of lithium metal counter electrode to sodium contamination in half-cell test with hybrid-ion electrolyte containing different cations. In this work, we have found that lithium metal electrodes in hybrid-ion electrolyte are unstable and Na + causes significant polarization. The polarization influences over potential and complex interface properties and thus reduces the accuracy of half-cell tests. To solve the problem, lithium difluoro(oxalato)borate (LiDFOB) with excellent film-forming properties was utilized as an additive of symmetrical batteries to form solid electrolyte interface (SEI) film. The adverse effect of Na + on the kinetics of hybrid-ion electrolyte was confirmed by regulating the SEI film on lithium metal electrode. The SEI film exhibits a selective effect on Li + and Na + and inhibits the interfacial transport of Na + , which significantly reduces the overpotential of the batteries and the interface migration impedance and also improves the stability of lithium counter electrode. Lithium metal with stable interfacial properties in the presence of LiDFOB is a reliable counter electrode that resists sodium contamination in half-cell test. Graphical abstract
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Baolei Li,Qingsong Cai,Jianmin Zhang,Kai Zhang,Zongmin Zheng
The lithium metal batteries (LMBs) using Li metal as the anode are becoming one of the representatives of next-generation high-energy–density batteries. However, uneven deposition and stripping of Li usually cause capacity loss during cycling. To address these issues, NO 3 − intercalated LiAl layered double hydroxides (LiAl-LDHs) nanosheets were used as novel solid additives for conventional carbonate electrolytes. The abundant Li + transport pathways brought by LiAl-LDHs and the interlayer NO 3 − in LiAl-LDHs are beneficial to the uniform concentration distribution of Li + and high-quality solid electrolyte interface (SEI), thereby achieving stable deposition/stripping of Li. The assembled Li||Li symmetric cell was cycled stably for 500 h at a current density of 0.5 mA cm −2 . The Li||LFP(LiFePO 4 ) full cell had a capacity retention of 90 % after 800 cycles at 1C. Even at a high operating temperature of 50 °C, the Li||Li symmetric cells and Li||LFP full cells can still obtain steady charging-discharging performances.
研究领域:
材料科学
·
电化学
✓ 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）