Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 25
·12012-12017
·
IF 9.931
Lina Gao,Juner Chen,Yaqin Liu,Yusuke Yamauchi,Zhenguo Huang,Xueqian Kong
Stabilizing the reactive metal anode is a critical challenge for the development of next-generation alkali metal batteries. This work demonstrates that sodium-difluoro(oxalato)borate (NaDFOB)-based carbonate-ester electrolytes have excellent compatibility with the anode in sodium metal batteries, enabling high rate performance and long cycle life. The NaDFOB-based electrolytes possess favourable electrochemical stability and effectively passivate the Na metal anode by forming a compact, robust and conductive solid-electrolyte interphase (SEI) layer. Quantitative nuclear magnetic resonance (NMR) measurements of electrolyte solvents indicated that the SEI layer forms mainly in the initial cycles, and it prevents further solvent degradation. Solid-state NMR and X-ray photoelectron spectroscopy studies revealed the chemical composition of the NaDFOB-derived SEI film, which includes a mixed phase consisting primarily of sodium diborate, tetrafluoroborate and carbonate. The formation of such a composite SEI rich in borate and tetrafluoroborate provides robust structural and chemical stability, and facilitates fast ion transport for uniform Na stripping/plating.
研究领域:
化学
·
材料科学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Zongzhe Liu,Shaobo Ma,Xue Mu,Renlong Li,Geping Yin,Pengjian Zuo
A silicon anode with ultra-high specific capacity has motivated tremendous exploration for high-energy-density lithium ion batteries while it still faces serious issues of irreversible lithium loss, unstable electrode electrolyte interface (SEI), and huge volume expansion. Prelithiation is a crucial technology to alleviate the harm of active lithium loss of silicon-based full-cell systems. Herein, we reported a cathode prelithiation method using Li2S-PAN as a lithium “donor”, which was synthesized via chemical reaction between sulfurized polyacrylonitrile and Li-biphenyl complex. The Li2S-PAN with an initial charging capacity of 668 mAh g–1 (2.5–4.0 V) is loaded on the LiFePO4 electrode, and the LiFePO4/Li2S-PAN composite electrode displays a high initial charge capacity of 206 mAh g–1, which is 22.3% higher than the pristine LiFePO4. With a silicon/graphite/carbon (Si/G/C) composite anode, the Si/G/C||LiFePO4/Li2S-PAN full cell exhibits a reversible capacity of 123 and 107 mAh g–1 in the 1st and 10th cycle, which is 15.5 and 24.5% higher than the Si/G/C||LiFePO4 battery, respectively. The SEI layer of the silicon anode in the Si/G/C||LiFePO4/Li2S-PAN cell contains abundant conductive LiF species, which can enhance the interfacial stability and reaction kinetics of the cells. The proposed cathode prelithiation process is compatible with the industrial roll-to-roll electrode preparation process, exhibiting a promising application prospect.
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
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
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
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
Energy Storage Materials
·
2017
·
IF 0
Liping Wang,Lei Zhang,Qingji Wang,Wenjun Li,Bo Wu,Weishang Jia,Yuehui Wang,Jingze Li,Hong Li
Lithium metal is a Holy Grail anode for high energy density lithium ion batteries . While, its high chemical reactivity and high tendency to form dendrites hinder its wide applications. Here, in this study, we stabilize lithium metal by engineering an artificial SEI layer, namely fabricating a conformal nano-meter thickness amorphous Al 2 O 3 thin film via magnetron sputtering technique on its surface. The obtained Al 2 O 3 modified Li metals present robust chemical surface stability and effectively restrain the dendrite growth. 20 nm-thick Al 2 O 3 film modified lithium metal in an all-solid-state battery Li/PEO-LiTFSI/Li ensures a cycle life of 660 h at a current density of 0.1 mA/cm 2 . Contradicting to a traditional belief of lithium plating at the current collector side via crossing the Al 2 O 3 film, it directly plates on the Al 2 O 3 film next to the separator side. Al 2 O 3 film plays a crucial role as a “surfactant” in inducing a layer-by-layer film growth mode.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Weitao Jing,Kunyang Zou,Xin Dai,Junjie Sun,Qiang Tan,Yuanzhen Chen,Yongning Liu
Lithium metal has been considered one of the most ideal anode materials for batteries due to its ultrahigh theoretical capacity and energy density . However, the unstable SEI layer and the growth of Li dendrites cause poor cycling performance and even safety hazards, which also severely restrict the commercial application of Li metal batteries . In this paper, a Li-In alloy anode was designed and prepared by mechanical rolling of both Li and In pure metal foils together. Three-dimensional Li-In alloy network structures are formed by mechanical alloying during rolling, and the 3D Li-In alloy structure not only possesses strong lithium affinity but also possesses more interface between the Li matrix and the second phase formed in mechanical alloying, which can promote rapid diffusion at the interface and uniform deposition of lithium ions . As a result, the Li-In electrode shows an extremely low overpotential of approximately 35 mV at a high current density of 5 mA cm −2 during the lithium plating/stripping experiment. In addition, the battery revealed a higher discharge capacity of 295 mAh/g at 0.05 C and capacity retention of 80 % after 150 cycles when the Li-In alloy was used as the anode electrode in a cell with Li 1.2 Ni 0.2 Mn 0.6 O 2 as the cathode. The Li-In alloy can also be used as anode of Li-S battery, the result showed that the capacity decay rate was reduced from 0.22 % to 0.1 % after 200 cycles without any decoration treatment of S cathode except conductive carbon. This work verified that indium in the Li-In alloy can effectively protect the lithium anode and provides an idea for the practical application of lithium metal batteries.
研究领域:
材料科学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
COMPOSITES PART B-ENGINEERING
·
2022
·
IF 11.322
Kaizhao Wang,Jin Hu,Tianyou Chen,Kaijun Wang,Zhongshan Deng,Jun Wu,Yongjin Feng,Qingming Chen,Weijun Zhang
Gallium-based liquid alloys that exhibit high capacity and self-healing properties have been demonstrated to be promising cathodes for room temperature liquid metal batteries (RTLMBs). However, the electrochemical performances of these alloys are poor due to severe volume expansion and an unstable solid electrolyte interface layer during the lithiation process. Here, a sol-gel strategy was performed to construct yolk-shell structure nanodroplets (eGaSn@Void@SiO 2 ) that contain sufficient void space by amorphous silicon oxide , which generated a liquid metal electrode with a high performance. The amorphous SiO 2 shells not only play an important role in building stable SEI films, providing efficient electron/ion conduction channels and preventing agglomeration of active substances, but exhibit good elastic behavior during charging/discharging. Due to the appropriate voids in the yolk-shell structure, the eGaSn nanodroplets can expand freely without breaking or disrupting the electrode structure ; thus, the resulting eGaSn@Void@SiO 2 NDs exhibited high capacities of 538, 454, and 338 mA h g −1 at current rates of 0.2, 1 and 5 C, respectively. No obvious decay was observed with more than 500 cycles and a capacity of 377 mA h g −1 at 2 C. Interestingly, the density functional theory (DFT) calculations revealed that the effective chemisorption between the discharge products and SiO 2 provides sufficient electrical contact sites with a significant drop in electrochemical impedance during cycling. The causes of the superior electrodes performance were investigated in depth using in situ X-ray diffraction and theoretical calculations. Our rational design may shed unprecedented light on the development of liquid alloy-based cathodes for high-performance RTLMBs.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Tianqi Jia,Geng Zhong,Sirong Lu,Xiaolong Ren,Yao Lv,Nanrui Li,Rui Yin,Guohuang Kang,Kangning Cai,Feiyu Kang,Yidan Cao
Active lithium loss, which is caused by parasitic reactions due to the instability of solid electrolyte interphase (SEI) on the anodes, results in fast capacity fade of batteries. Constructing robust SEI layer is an effective way to reduce active lithium loss. Herein, we propose a AgF-coated separator (AgF-CS) to facilitate robust LiF-rich SEI on the anode during initial cycle. Electrochemical analysis and microstructure investigations confirm the formation of the LiF-rich SEI on the anode induced by the fluoride-containing coating layer. The fluoride-containing interfacial layer not only effectively enhances the reversible capacity of the SiO anode even under lean electrolyte (14 μL mAh −1 ) condition, but also prolongs the cycling life of lithium metal batteries by reducing the consumption of electrolyte and active lithium. The initial Coulombic efficiency (ICE) of LiFePO 4 ||SiO full cell is increased from 43.68 % to 84.18 % with pretreatment by AgF-CS. As a result, the reversible capacity of LiFePO 4 ||SiO full cell is increased by ∼124 % in contrast with that of the unmodified one. The strategy proposed here, benefiting from the simple manufacture, provides a feasible way to alleviate active lithium loss and elevate energy density of rechargeable lithium batteries.
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
·
2022
·
IF 16.744
Xin Hou,Tianyu Li,Yanling Qiu,Mingqin Jiang,Qiong Zheng,Xianfeng Li
Electrolyte plays an important role in conducting sodium ions and carrying out chemical/electrochemical reactions. However, the impact mechanism of microscopic solvation structure remains vague but is significant for the electrolyte design. Here we reveal that the inner relationship between solvation structure and electrochemical reaction is manifested intuitively by manipulating the anions in the solvated shell, which determines Na storage kinetics and SEI evolution process. The result elucidates the weak coulomb interaction between PF 6 − and Na + could promote Na + transport number in bulk liquid and Na storage kinetics. And it could induce PF 6 − to reduce preferentially and facilitate additive to enter solvation structure, thereby forming a thin&compact&protective SEI with layered morphology. The excellent SEI would protect anode effectively, inhibiting decomposition of solvents and improving battery performances. As expected, 5 Ah Na 3 V 2 (PO 4 ) 3 -hard carbon pouch-type batteries with well-matched PF 6 − -based electrolyte display a high specific energy of 129 Wh kg −1 , a superior rate capability with capacity retention of 90 % at 5 C and cycling stability with retention of 86.82 % at 1 C after 700 cycles.
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）