INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Li Fang,Wang Sun,Wenshuo Hou,Yuqiong Mao,Zhenhua Wang,Kening Sun
Solid-state polymer electrolytes (SPEs) complexing a plasticizer is a valid strategy to improve the poor ionic conductivity of SPEs at ambient temperature. In this study, a quasi-SPE based on a polyurethane matrix (QSPE-PU) is constructed by regulating the contents of bis(trifluoromethanesulfonyl) imide (LiTFSI) salt and N,N-dimethylformamide (DMF) and shows high performance in ambient-temperature rechargeable lithium batteries. Highly concentrated LiTFSI is designed to anchor DMF, decreasing the free solvent molecules in the QSPE to improve the stability with lithium metal. Meanwhile, DMF can fully dissociate the highly concentrated LiTFSI, providing more carriers. The prepared QSPE-PU40 shows a high ionic conductivity of 1.12 × 10–4 S cm–1 at ambient temperature since DMF not only provides more carriers but also enhances the movement of the polymer segments and lowers the energy barrier of lithium ion migration. Density functional theory calculations further prove that DMF facilitates the conduction of lithium ions in the QSPE system. QSPE-PU40 shows good compatibility with the lithium metal electrode by forming a stable solid electrolyte interphase during lithium plating/stripping processes. The lithium ferrophosphate (LFP)/QSPE-PU40/Li battery exhibits a high specific capacity of 138 mA h g–1 with remarkable cycling stability at 0.5 C and 30 °C (94% capacity retention after 800 cycles). More impressively, the pouch cell based on QSPE-PU40 delivers good flexibility and high safety. Such a QSPE is expected to provide an effective strategy where SPEs are applied in solid-state lithium batteries at ambient temperature and even flexible batteries for next-generation wearable devices.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2026
·
IF 5.8
Jun Seo,Mohammad Nasir,Taeho Moon,Hee Jung Park
Low ionic conductivity and low Li⁺ transference numbers limit the practical application of polyethylene oxide (PEO)-based polymer solid electrolytes, arising from PEO semi-crystallinity and poor lithium salt dissociation at ambient conditions. Here, we systematically investigate the size-dependent role of CeO 2 fillers by incorporating nanosized (∼5 nm) and submicron particles into PEO-LiTFSI electrolytes. The nanosized CeO 2 , enriched with surface oxygen vacancies and high specific surface area, simultaneously suppresses PEO crystallinity and provides abundant Lewis acid sites that immobilize TFSI⁻ via Lewis acid-base interactions, increasing the mobile Li + carrier concentration. As a result, the nanosized CeO 2 -based composite electrolyte exhibits an ionic conductivity of 5.95 × 10 –5 S/cm at room temperature (2.4 × higher than pristine PEO) and a Li⁺ transference number of 0.30, nearly fourfold higher than the filler-free system (0.08). In addition, it delivers a widened electrochemical stability window of ∼4.9 V, a high critical current density of 0.8 mA/cm², and stable Li||Li symmetric cycling over 600 h, substantially outperforming both the submicron CeO 2 -based composite and the filler-free electrolytes. Download: Download high-res image (522KB) Download: Download full-size image
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DOI
高影响因子
GIANT
·
2021
·
IF 0
Zekun Zhou,Ruike Zou,Zhen Liu,Peng Zhang
Residual solvent in polymer electrolytes recently has attracted great attention since it influences the performance and safety of the polymer-electrolyte based batteries and electric vehicles. In this work, we did a systematic study of exploring the role of the residual solvent in lithium-ion secondary battery electrolyte beyond the traditional understanding of plasticizing effect, based on the typical polymer electrolyte system of polyethylene oxide/tetrahydrofuran/lithium bis(trifluoromethanesulfonyl)imide (PEO/THF/LiTFSI). A series of complementary characterization techniques, i.e., small-angle neutron scattering (SANS), wide-angle X-ray scattering (WAXS), Raman, infrared, nuclear magnetic resonance, thermogravimetric analysis and electrochemical impedance spectroscopy, were applied to decipher the structure-function relationship. We found that the PEO/LiTFSI hybrid formed a complex with the THF residue, which was further confirmed by the Gaussian simulation. By using the oxygen-free solvent, acetonitrile, as a reference, we demonstrated that THF provided ambient oxygen bonding sites among PEO and LiTFSI, which leaded to PEO/LiTFSI/THF clusters and endowed the hybrid a ionic conductivity value of 1.1 × 10 −4 S cm −1 at 30 °C. The battery showed a discharge capacitance of 905 mAh g −1 at 0.1C in a Li-S cell. Moreover, both ionic conductivity and cell performance deteriorate significantly with vigorous drying of the polymer electrolyte membrane in vacuum oven at 120 °C and argon-purged glove box at room temperature, although there are still around 10 wt% THF residues found in the dried membranes. It seems to be that the vigorous drying caused damage to the PEO/LiTFSI/THF clusters and the ion conductive network, especially around the electrode/electrolyte interfaces. Our findings shed light on improving the ionic conductivity of polymer electrolyte for lithium-ion secondary battery by carefully tailoring the solvent residue.
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DOI
ChemistryOpen
·
2020
·Vol. 9
·期 6
·713-718
·
IF 2.37
Wang Lyu,Guoqiang He,Ting Liu
All-solid-state polymer lithium-ion batteries are ideal choice for the next generation of rechargeable lithium-ion batteries due to their high energy, safety and flexibility. Among all polymer electrolytes, PEO-based polymer electrolytes have attracted extensive attention because they can dissolve various lithium salts. However, the ionic conductivity of pure PEO-based polymer electrolytes is limited due to high crystallinity and poor segment motion. An inorganic filler SiO 2 nanospheres and a plasticizer Succinonitrile (SN) are introduced into the PEO matrix to improve the crystallization of PEO, promote the formation of amorphous region, and thus improve the movement of PEO chain segment. Herein, a PEO 18 −LiTFSI−5 %SiO 2 −5 %SN composite solid polymer electrolyte (CSPE) was prepared by solution-casting. The high ionic conductivity of the electrolyte was demonstrated at 60 °C up to 3.3×10 −4 S cm −1 . Meanwhile, the electrochemical performance of LiFePO 4 /CSPE/Li all-solid-state battery was tested, with discharge capacity of 157.5 mAh g −1 at 0.5 C, and capacity retention rate of 99 % after 100 cycles at 60 °C. This system provides a feasible strategy for the development of efficient all-solid-state lithium-ion batteries. Graphical All-solid-state polymer lithium-ion batteries are ideal choice for the next generation of rechargeable lithium-ion batteries due to their high energy, safety and flexibility. The ionic conductivity of pure PEO-based polymer electrolytes are limited by high crystallinity and poor segment motion. In this work, an inorganic filler and a plasticizer have been introduced into the PEO matrix to improve the crystallization and promote the formation of amorphous region, and thus improve the movement of PEO chain segments. This work provides a feasible strategy for the development of all-solid-state lithium-ion battery.
研究领域:
材料科学
·
电化学
·
储能技术
·
高分子科学
·
锂离子电池
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2020
·
IF 4.473
Tao Wei,Zao-Hong Zhang,Zhi-Meng Wang,Qi Zhang,Yu-sheng Ye,Jia-Hao Lu,Zia ur Rahman,Zhi-Wei Zhang
Solid composite electrolytes (SCEs) are regarded as an effective solution to ensure safety and enhance the energy density of lithium-based batteries. This work reports an ultrathin SCE membrane (∼ 15 μm) based on Li6.4La3Zr1.4Ta0.6O12/PVDF-HFP/LiTFSI/succinonitrile; it not only possesses good ionic conductivity (6.53 × 10–4 S cm–1 with a little amount of liquid electrolyte) at 30 °C and a satisfactory lithium ion transfer number (0.55 without electrolyte), but also exhibits excellent thermal and mechanical properties. A symmetric cell with SCE succinonitrile-10% (SN-10%) can be continuously cycled without short circuit at 0.2 mA cm–2 for about 340 h. Moreover, a high reversible discharge capacity of 150.2 mAh g–1 at 0.5 C was maintained by the cell (LiFePO4/SCE SN-10%/Li) after 269 cycles at room temperature. Notably, a capacity of about 100 mAh g–1 at 5 C was also obtained. This work might guide the improvement of future solid-state lithium/sodium metal batteries and lithium–sulfur batteries, even for wearable flexible batteries.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2024
·Vol. 171
·期 5
·050534
·
IF 3.1
Yi Zou,Yaozhong Chen,Tao Jiang,Songxue Shao,Mingjing Xiao,Yuetong Lv,Yuting Wang,Lvjin Gao,Li Chen,Wentao Zhao
It is popular to choose the cubic phase Li7La3Zr2O12(c-LLZO) to synthesize the PEO-based complex membrane in all-solid-state battery. In this work, Ba/Nb elements were selected to achieve Li6.75La3Zr1.75Nb0.25O12 (LLZNO) and Li7La2.75Ba0.25Zr1.75Nb0.25O12 (LLBZNO) with high ion conductivity, which effectively enhance the electrochemical properties of the complex solid membrane and the all-solid-state battery. The higher ion mobility of LLBZNO compared to that of LLZNO and LLZO is calculated by ab-initio molecular dynamics (AIMD) simulation and further confirmed by experiments. Results show that the cubic phase of LLBZNO is more stable than that of LLZNO. The complex membrane of LLBZNO@ polyethylene oxide (PEO) (CPE-2-x wt%) exhibits the better electrochemical properties than LLZNO@PEO (CPE-1-x wt%) complex membrane. In detail, the CPE-2–10 wt% has the outstanding lithium transfer number ({t}_{{{Li}}^{+}}) of 0.63, as well as the excellent compatibility with lithium metal anode. In addition, at 0.1 mAcm−2, the lithium/CPE-2–10 wt%/lithium symmetric cell remains stable after 1000 h. It is LLBZNO that makes LLBZNO@PEO composite polymer electrolyte(CPE) the potential for the application in all-solid-state lithium battery.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
·
2019
·
IF 5.162
Yumei Zhou,Fengrui Zhang,Peixin He,Yuhong Zhang,Yiyang Sun,Jingjing Xu,Jianchen Hu,Haiyang Zhang,Xiaodong Wu
Succinonitrile (SN)-based polymer plastic crystal electrolytes (PPCEs) have attracted considerable attention as solid-state electrolytes owing to their high ionic conductivities similar to those of liquid electrolytes, excellent contacts with the electrodes, and good mechanic properties. As a crucial property of a solid-state electrolyte, the ionic conductivity of the PPCE directly depends on the interactions between the constituent parts including the polymer, lithium salt, and SN. A few studies have focused on the effects of polymer–lithium–salt and polymer–SN interactions on the PPCE ionic conductivity. Nevertheless, the impact of the lithium–salt–SN combination on the PPCE ionic conductivity has not been analyzed. In particular, tuning of the lithium-salt–SN interaction to fabricate a subzero PPCE with a high low-temperature ionic conductivity has not been reported. In this study, we design and fabricate five PPCE membranes with different weight ratios of LiN(SO 2 CF 3 ) 2 (LiTFSI) and SN to investigate the effect of the LiTFSI–SN interaction on the PPCE ionic conductivity. The ionic conductivities of the five PPCEs are investigated in the temperature range of –20 to 60 °C by electro-chemical impedance spectroscopy. The interaction is analyzed by Fourier-transform infrared spectroscopy, Raman spectroscopy, and differential scanning calorimetry . The LiTFSI–SN interaction significantly influences the melting point of the PPCE, dissociation of the LiTFSI salt, and thus the PPCE ionic conductivity. By tuning the LiTFSI–SN interaction, a subzero workable PPCE membrane having an excellent low-temperature ionic conductivity (6 × 10 −4 S cm –1 at 0 °C) is obtained. The electro-chemical performance of the optimal PPCE is evaluated by using a LiCoO 2 /PPCE/Li 4 Ti 5 O 12 cell, which confirms the application feasibility of the proposed quasi-solid-state electrolyte in subzero workable lithium-ion batteries.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF POLYMER SCIENCE
·
2021
·Vol. 39
·期 8
·975-983
·
IF 3.603
Li Hui-Xian,Hou Lei,Wu Pei-Yi
The time-resolved attenuated total reflectance-Fourier transform infrared (ATR-FTIR) spectroscopy is employed to investigate the transport mechanism of gel electrolytes by monitoring the diffusion behavior of propylene carbonate-lithium bis(trifluoromethylsulfonyl)imide (PC-LiTFSI) solution through poly(vinylidene fluoride- co -hexafluoropropylene) (P(VDF-HFP)) films. Fickian behavior has been observed for both TFSI − and PC. Higher temperature leads to faster diffusion of TFSI − and PC, which could be related to the increased free volume in P(VDF-HFP) matrix and rapid molecular movements upon heating. Various molecular interactions among LiTFSI, PC and P(VDF-HFP) have been recognized. During the diffusion process, PC molecules, in the form of small clusters, can firstly diffuse through the P(VDF-HFP) film and interact with P(VDF-HFP) by dipole-dipole interaction, acting as the plasticizer. Then, Li + diffuses into P(VDF-HFP) with the help of ion-dipole interactions between Li + and C-O of PC. Meanwhile, TFSI − diffuses through the polymer matrix in solvation states. In addition, slight ion-dipole interactions between Li + and P(VDF-HFP) have been observed as well. Results in this work contribute to a better understanding of transport process in gel polymer electrolytes for lithium-ion batteries and support the development of improved gel polymer electrolytes by rationally regulating molecular interactions.
研究领域:
高分子化学
·
电化学
·
能源材料
·
锂离子电池
·
光谱分析
✓ 已验证
DOI
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-11
·
IF 17.694
Sun Zongjie,Xi Kai,Chen Jing,Abdelkader Amor,Li Meng-Yang,Qin Yuanyuan,Lin Yue,Jiang Qiu,Su Ya-Qiong,Vasant Kumar R.,Ding Shujiang
Ionic-conductive polymers are appealing electrolyte materials for solid-state lithium-based batteries. However, these polymers are detrimentally affected by the electrochemically-inactive anion migration that limits the ionic conductivity and accelerates cell failure. To circumvent this issue, we propose the use of polyvinyl ferrocene (PVF) as positive electrode active material. The PVF acts as an anion-acceptor during redox processes, thus simultaneously setting anions and lithium ions as effective charge carriers. We report the testing of various Li||PVF lab-scale cells using polyethylene oxide (PEO) matrix and Li-containing salts with different anions. Interestingly, the cells using the PEO-lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) solid electrolyte deliver an initial capacity of 108 mAh g −1 at 100 μA cm −2 and 60 °C, and a discharge capacity retention of 70% (i.e., 70 mAh g −1 ) after 2800 cycles at 300 μA cm −2 and 60 °C. The Li|PEO-LiTFSI|PVF cells tested at 50 μA cm −2 and 30 °C can also deliver an initial discharge capacity of around 98 mAh g −1 with an electrolyte ionic conductivity in the order of 10 −5 S cm −1 .
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2024
·
IF 2.7
Wei Liu,Shilong Cai,Hefeng Zhang,Yifu Huang
The presence of well-conductive polydimethylsiloxane (PDMS)-based ionogel has changed the stereotype of PDMS of being an insulator, owing to continuous ionic liquid (IL) phase with superior ionic conductivity. However, the sacrifice on the transparency of ionogel often occurs if increasing IL content, and to overcome the immiscibility between nonpolar PDMS and polar IL is still regarded as a considerable challenge today. Herein a new strategy to prepare a transparent, highly conductive PDMS-based ionogel with high IL content is proposed, using a “composite” surfactant of KF-6017 and LiTFSI. Benefited from unique microphase separation during gel formation, the optimal ionogel of IG 70%–1%–1% can possess excellent transparency (>95%, ~200 μm) with IL content of 70%, while owning ionic conductivity of 3.28 mS/cm and tensile property of 100 kPa. A new mechanism on the conductivity of ionogel is proposed by the molecular simulation. The ionogel can be suitable for applying as electrolyte (B) and a polymer binder for active carbon powders (as electrode A). As a result, the assembled electrochemical double-layer capacitor (A/B/A) can be flexible accompanied with excellent electrochemical performance, which exhibits a promising future for flexible electronics and wearable devices.
研究领域:
材料科学
·
化学工程
·
柔性电子学
✓ 已验证
产品关联
DOI
高影响因子
ACS Omega
·
2026
·Vol. 11
·期 34
·50883-50891
·
IF 5.2
Kang Hongrui,Ma Weiye,Hofmann Jan P.,Gao Zhonghui
Composite solid polymer electrolytes (CSPEs) with inorganic
fillers
are of great interest for advanced all-solid-state lithium–metal
batteries (ASSLMBs), enabling high energy density and enhanced safety.
Despite increasing interest, the effects of different inorganic fillers
on the interface between CSPEs and the lithium metal anode (LMA) remain
not fully understood. Herein, we systematically study the contact
behavior between the LMA and CSPEs containing PEO, LiTFSI, as well
as oxide- (Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 ), sulfide- (Li 6 PS 5 Cl), and halide-based
(Li 3 InCl 6 ) fillers by evaporating lithium metal
stepwise onto CSPE thin films under ultrahigh vacuum conditions, followed
by in-system X-ray photoelectron spectroscopy (XPS)
analysis. XPS results demonstrate that halide-based fillers can facilitate
the formation of electron-rich Li–O and Li–S species
at the interfaces, acting as a passivation layer, which can prevent
further decomposition of the CSPE and thus improve interfacial stability.
In contrast, the incorporation of oxide- and sulfide-based fillers
does not promote the interfacial reactions. Impedance spectroscopy
as a function of resting time also shows that the incorporation of
a halide-based filler reduces the CSPE/LMA interfacial impedance,
which is beneficial for increasing the critical current density for
lithium dendrite formation. The incorporation of active inorganic
fillers to induce protective interphases offers a novel strategy for
interfacial engineering of ASSLMBs.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2022
·
IF 9.794
Yuanduo Qu,Xia He,Jinling Hu,Lianfeng Duan,Junkai Wang,Siqi Liao,Fushen Lu
The combination of solar cells and rechargeable batteries has been confirmed as a new strategy for the development of solar energy utilization. However, the high charging voltage of Li-ion battery (3.0–4.2 V) and incompatible electrolyte with solar cell is adverse to the combination of photo-assisted rechargeable battery (PRB). In this work, Li–S battery as an energy storage unit is combined with dye-sensitized solar cell to form an integrated three-electrode photo-assisted rechargeable Li–S battery (PRSB). The compatible C/S electrode provides a bridge for realizing the bi-function of photoelectric conversion and storage. In contrast to the dual electrolytes in the previously reported PRBs, lithium bis((trifluoromethyl)sulfonyl)azanide (LiTFSI), namely the highly compatible mono-electrolyte in our newly designed PRSB with three-electrode, facilitates the charge separation and enhances the capacity and stability of integrated photo-assisted rechargeable battery. With the compensation of photogenerated carrier , the charge voltage of PRSB drops 0.12 V and the discharge capacity increases to 885 mAh g −1 under solar charging, indicating that the integrated device is promising to save electric energy and improve the performance of PRBs.
研究领域:
能量存储
·
太阳能
·
电池技术
·
光电化学系统
✓ 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）