CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yali Liu,Youlong Xu
The application of solid polymer electrolytes (SPEs) has been impeded by the low ionic conductivity, narrow oxidation potential and poor mechanical strength. Herein, we designed a novel in-situ PVDF-HFP/Poly 1,3-dioxolane (PDOL) polymer electrolyte with dual-salts and functional plasticizers of succinonitrile (SN)/fluoroethylene carbonate (FEC). One of the dual-salts, Lithium difloro(oxalato)borate (LiDFOB), could initiate the polymerization of DOL in-situ in the porous PVDF-HFP host to improve the interfacial compatibility. SN is beneficial to the improvement of ionic conductivity and the stability of high voltage cathodes, while the FEC can generate the LiF-rich SEI on Li metal anode. The PVDF-HFP host can further restrict the motion of anion and increase the strength of the SPE. Therefore, the as-obtained SPE exhibits a thin thickness of ∼ 32 μm, high ionic conductivity of 1.06 × 10 −4 S cm −1 at room temperature, an enlarged electrochemical window of 5.86 V versus Li/Li + and high lithium-ion transference number t Li+ of 0.72. Benefited from the synergetic effect, the Li/LiFePO 4 cell delivers a high initial capacity of 141.7 mAh g −1 at 2C with a capacity retention of 94.99% after 1000 cycles. This three-dimensional porous film-derived in-situ polymer electrolytes provide a new sight and simple strategy for designing polymer electrolytes, exhibiting attractive potential in flexible and high-energy–density solid-state batteries.
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高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 30
·16087-16094
·
IF 14.511
Cun Song,Zhengang Li,Jun Peng,Xiaohong Wu,Hao Peng,Shiyuan Zhou,Yu Qiao,Hui Sun,Ling Huang,Shi-Gang Sun
Solid polymer electrolytes (SPEs) could effectively enhance energy density and safety of Li-metal batteries (LMBs). Poly(ethylene oxide) (PEO)-SPEs exhibit excellent properties at elevated temperature (>70 °C), while their insufficient ionic conduction at room temperature yields nonnegligible mass transfer polarization. Such a polarization of SPEs in LMBs will lead to huge capacity loss, affect rate performance, cause Li dendrite growth that initiates safety problems, and significantly limit the battery lifespan. Herein, we have developed a method for improving the transfer efficacy of Li+ in PEO electrolyte through the construction of composite PEO with Li6.4La3Zr1.4Ta0.6O12 (LLZTO)/fluorinated carbonate (FEC) and succinonitrile (SN) (denoted as PLFS). By means of the decomposition reaction between LLZTO and FEC, interfacial compatibility between LLZTO and PEO has been improved, and fluorinated oligomers generated in the decomposition of FEC can simultaneously fix anions by the ‘fluorous effect’. Furthermore, SN with a lower Gutmann donor number is used to composite with PEO/FEC/LLZTO to weaken the strong complexation between Li+ and PEO. The construction of a fast Li+ transfer channel as well as the weakened interaction of Li+ to PEO is achieved, which facilitates the migration of Li+ of PEO-SPEs. Benefiting from the above design, composite PLFS-SPEs present an excellent Li+ transfer efficacy that is 41 times higher than that of pure PEO-SPEs, and significantly enhances rate performance and cycling life of LMBs. The Li/PLFS-SPEs/Li symmetric battery demonstrates a lifespan of more than 1100 h at room temperature. When PLFS-SPEs are applied in LMBs, the Li/PLFS-SPEs/LiFePO4 battery can maintain nearly 80% of its initial capacity after 700 cycles at 1C.
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ACS Nano
·
2022
·
IF 18.027
Wanbao Wu,Yihong Liang,Deping Li,Yiyang Bo,Dong Wu,Lijie Ci,Mingyu Li,Jiaheng Zhang
The development of electrolytes with high safety, high ionic conductivity, and the ability to inhibit lithium dendrites growth is crucial for the fabrication of high-energy-density lithium metal batteries. In this study, a ternary eutectic electrolyte is designed with LiTFSI (TFSI = bis(trifluoromethanesulfonyl)imide), butyrolactam (BL), and succinonitrile (SN). This electrolyte exhibits a high ion conductivity, nonflammability, and a wide electrochemical window. The competitive solvation effect among SN, BL, and Li+ reduces the viscosity and improves the stability of the eutectic electrolyte. The preferential coordination of BL toward Li+ facilitates the formation of stable solid electrolyte interphase films, leading to homogeneous and dendrite-free Li plating. As expected, the LiFePO4/Li cell with this ternary eutectic electrolyte delivers a high capacity retention of 90% after 500 cycles at 2 C and an average Coulombic efficiency of 99.8%. Moreover, Ni-rich LiNi0.8Co0.1Al0.1O2/Li and LiNi0.8Co0.1Mn0.1O2/Li cells based on the modified ternary eutectic electrolyte achieve an outstanding cycling performance. This study provides insights for understanding and designing better electrolytes for lithium metal batteries and analogous sodium/potassium metal batteries.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yue Ma,Qifang Sun,Su Wang,Ying Zhou,Dawei Song,Hongzhou Zhang,Xixi Shi,Lianqi Zhang
Favorable interface is essential for the implementation of high energy density and high safety solid-state lithium metal battery (SSLMB). The in-situ transformation of electrolyte from liquid to solid-state is of great significance for the compatibility of interface. Herein, an in-situ polymerized glycerin triglycidyl ether (PGTE) solid polymer electrolyte (SPE) featuring excellent ion transfer capability, superior interfacial compatibility and cross-linked structure is developed by the initiation of optimal LiDFOB following cationic catalytic mechanism. Ionic conductivity of 4.16 × 10 -4 S cm −1 is achieved at 60 °C due to the superiority of oxyethylene repeating units (C–C-O/C-O-C), and a discharge capacity of 135.2 mAhg −1 is obtained after 200 cycles at 0.2C for LiFePO 4 (LFP)/PGTE/Li battery. More importantly, as a Li salt initiated SPE, the in-situ polymerization process of PGTE is firstly investigated via ex-situ FT-IR, the ring opening catalytic activity of Lewis acid on epoxide is evaluated and the order of LiDFOB＞LiPF 6 ＞AlCl 3 is revealed. Furthermore, the effect of in-situ prepared SPE on electrode/electrolyte interface is innovatively explored using in-situ electrochemical impedance spectroscopy (EIS). The stable interfacial passivation layer is generated at platform voltage and the maximum value of average diffusion coefficient is also obtained at the plateau.
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高影响因子
SOLID STATE IONICS
·
2021
·
IF 3.785
Ruohan Xie,Xuexian Yu,Zhoupeng Li,Qinghua Zhang,Jian Chen,Jianguo Lu,Yang Hou,Qinggang He,Yingwu Luo,Xiang Gao
The rapid development of wearable electronics demands for high-safety and stretchable lithium-ion batteries which are closer to the human skin, then accelerating the requirement for all-solid-state electrolytes with high stretchability and ion conductivity. Here, we proposed a decoupling strategy to effectively overcome the theoretical tradeoff between mechanical properties and ion conductivity of all-solid-state polymer electrolytes . The prepared stretchable all-solid-state polymer electrolyte (SSPE) via UV polymerization exhibits outstanding elastic tensile properties with elongation at break around 160.38%. The most interesting thing is that the SSPE membrane maintain high ion conductivity under external stress, the ion conductivity is 4.65 × 10 −4 S cm −1 (0% strain) and 4.24 × 10 −4 S cm −1 (75% strain) at room temperature . In addition, the SSPE membrane shows an excellent electrochemical stability window up to 5.2 V ( vs. Li + /Li). The practicality of the SSPE was also investigated, including cell performance, deformation tests and destruction experiments. Therefore, the reported design of decoupling dual-function networks provides a promising approach for creating all-solid-state polymer electrolytes with high safety for stretchable energy storage applications .
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高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2021
·Vol. 139
·期 16
·52001
·
IF 3.125
Shujian Zhang,Yang Lu,Kewu He,Xianghui Meng,Lanfang Que,Zhenbo Wang
To solve the issues of low ionic conductivity, poor interfacial stability, and weak mechanical strength in the current polymer electrolytes, herein, the UV curing method is proposed to in-situ polymerize the plastic crystal composite solid polymer electrolyte (S-PCCE). By using ethoxylated trimethylolpropane triacrylate (ETPTA) as polymerization monomer, in conjunction with the butadiene nitrile and other additives, the S-PCCE is prepared under ultraviolet light. The S-PCCE shows improved ionic conductivity than other solid electrolyte materials. The ionic conductivity at room temperature can reach 0.98 × 10 −3 S/cm, and it can reach 2.8 × 10 −3 S/cm at 55°C, which is beneficial to achieve high battery performance. The LiFePO4/S-PCCE/Li battery has a high initial discharge specific capacity of 150.4 mAh/g at 0.2C, and the highest discharge specific capacity can reach 162.5 mAh/g. Moreover, after 100 cycles, the battery can still maintain a high discharge specific capacity of 154.2 mAh/g, with a Coulomb efficiency of 98.4%. At the same time, the electrolyte has excellent high-temperature adaptability, and can still work stably at 55°C with improved ionic conductivity. The superior performance of this material indicates that the plastic crystal composite polyacrylate solid electrolyte based on UV curing method can be used to prepare a high-performance lithium-ion battery, and this technology can also be compatible with existing lithium-ion battery equipment.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Wei Wu,Zhenyao Wei,Jun Wang,Jian Shang,Man Wang,Shang-Sen Chi,Qingrong Wang,Leilei Du,Tian Zhang,Zijian Zheng,Yonghong Deng
Flexible solid-state batteries (FSSBs) are indispensable energy storage devices to fulfil the energy and safety requirements for future flexible applications. The bottlenecks of FSSBs are how to realize high energy density with competent ionic conductivity for room-temperature (RT) flexible applications. Here, the first fabrication of RT FSSB with high energy density is reported, which is realized by in situ integration of a 20-µm-thick hybrid polymer/ceramic/ionic liquid solid-state electrolyte (SSE) between the high energy combination of anode/cathode electrodes. The in situ electrode/electrolyte interfacial integration strategy provides an ultrathin SSE layer, ultralow resistance and superior flexibility, and the SSE guarantees both high ionic conductivity and good compatibility with high-energy cathode LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811). The fabricated Li 4 Ti 5 O 12 /NCM811 FSSB delivers super-low resistance approaching conventional liquid cells and excellent cycling stability up to 600 cycles at RT. The extension of anode to SiO x @graphite leads to a high theoretical energy density of 489.6 Wh kg −1 at material’s level, times higher than current options. In addition, the RT FSSB shows great flexibility, indicating a high performance application in future flexible electronics.
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高影响因子
Nano Energy
·
2020
·
IF 16.602
Wei Wu,Man Wang,Jun Wang,Zhenyao Wei,Tian Zhang,Shang-Sen Chi,Chaoyang Wang,Yonghong Deng
Solid-state lithium metal batteries (LMBs) receive increasing attentions worldwide due to their safety and high energy density . Herein, the practical application of conversion reaction-type transition metal oxides (TMOs, Fe 2 O 3 , Mn 2 O 3 or CuO) as Li-free cathodes for solid-state LMBs is demonstrated for the first time, employing poly(ethylene oxide) (PEO), lithium garnet Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 or Li 1.5 Al 0.5 Ge 1.5 (PO 3 ) 4 solid-state electrolytes (SSEs). The cathodes embody good interfacial compatibility with the SSEs, ensuring the excellent electrochemical performance of the TMOs/SSEs/Li solid-state cells. The as-prepared Fe 2 O 3 /PEO/Li cell measured at 60 °C delivers a high discharge capacity of 990 mAh g −1 at 10 mA g −1 , which is comparable to the Fe 2 O 3 liquid cell. When cycling at 200 mA g −1 , a stable capacity of 733 mAh g −1 is achieved at the 1,100 th cycle for the Fe 2 O 3 /PEO/Li cell, while the Fe 2 O 3 liquid cell only sustains 860 cycles until failure. In order to further demonstrate the application feasibility, stable cycling of the Fe 2 O 3 /PEO/Li cells with high mass loading of 2.83 mg cm −2 and thus high areal capacity of 1.67 mAh cm −2 or with limited Li usage (150% in excess) is preliminarily achieved. In addition, the Fe 2 O 3 /PEO/Li pouch cells are assembled, which exhibit satisfied electrochemical performance. Moreover, poly(vinylidene difluoride) (PVDF)-based solid polymer electrolye is employed to make the Fe 2 O 3 solid-state cell work at 30 °C successfully. These results convince the great promise of TMOs in future high-energy-density solid-state LMBs.
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Journal of Materials Chemistry A
·
2019
·Vol. 8
·期 4
·2066-2073
·
IF 10.733
Chuankai Fu,Yulin Ma,Shuaifeng Lou,Can Cui,Lizhi Xiang,Wei Zhao,Pengjian Zuo,Jiajun Wang,Yunzhi Gao,Geping Yin
Succinonitrile (SN)-based electrolytes are attractive due to their considerable ionic conductivity and high oxidative stability. However, the spontaneous chemical side-reactions between SN and Li-metal restrict the extensive applications of such electrolytes in next-generation advanced Li-metal batteries. Herein, we report a novel SN-based electrolyte SN–DLi–FEC which combines the dual-salt (lithium bis(trifluoromethane sulfonimide) (LiTFSI) and lithium difluoro(oxalato)borate (LiODFB)) and the fluoroethylene carbonate (FEC) additive. Compared with other SN-based electrolytes such as SN–SLi–FEC (single salt combined with FEC), SN–DLi–FEC can form a more stable and durable organic–inorganic composite SEI film rich in the B–F bond and LiF on the surface of the Li-metal anode. As a result, interfacial compatibility of the SN-based electrolytes and the Li-metal anode can be significantly enhanced. Moreover, SN–DLi–FEC shows high oxidation resistance, high ionic conductivity and good thermal stability. The LiCoO2 (LCO)/Li battery equipped with SN–DLi–FEC exhibits excellent electrochemical performances at room temperature (RT) and high temperature, and high thermal safety. The novel SN-based electrolyte prepared in this work could be a promising candidate providing better reliability and safety for the development of Li-metal batteries.
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高影响因子
Science Advances
·
2023
·Vol. 9
·期 43
·
IF 13.6
Wei Zhao,Yiwei Zheng,Meng Jiang,Tingting Sun,Aibin Huang,Lianjun Wang,Wan Jiang,Qihao Zhang
Ionic liquid–based ionogels emerge as promising candidates for efficient ionic thermoelectric conversion due to their quasi-solid state, giant thermopower, high flexibility, and good stability. P-type ionogels have shown impressive performance; however, the development of n-type ionogels lags behind. Here, an n-type ionogel consisting of polyethylene oxide (PEO), lithium salt, and ionic liquid is developed. Strong coordination of lithium ion with ether oxygen and the anion-rich clusters generated by ion-preferential association promote rapid transport of the anions and boost Eastman entropy change, resulting in a huge negative ionic Seebeck coefficient (−15 millivolts per kelvin) and a high electrical conductivity (1.86 millisiemens per centimeter) at 50% relative humidity. Moreover, dynamic and reversible interactions among the ternary mixtures endow the ionogel with fast autonomous self-healing capability and green recyclability. All PEO-based ionic thermoelectric modules are fabricated, which exhibits outstanding thermal responses (−80 millivolts per kelvin for three p-n pairs), demonstrating great potential for low-grade energy harvesting and ultrasensitive thermal sensing.
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PubMed
高影响因子
POLYMER
·
2023
·
IF 4.6
Xiaoqing Tan,Xiang Ke,Keliang Wang,Kun Zou,Yong Zeng,Rengui Xiao
Solid polymer electrolytes are widely applied in lithium metal batteries owing to good flexibility and machinability . However, monolayer polymer electrolyte are difficult to simultaneously satisfy the interfacial contact with the cathode and Li anode. Herein, the dual-layer composite solid polymer electrolyte with polypropylene film (CSPE@PP) are designed to promote the interfacial compatibility between the solid electrolytes and electrodes. The X-ray photoelectron spectroscopy (XPS) results confirm that poly (vinylidene fluoride-co-hexafluoropropylene (PVDF-HFP) can react with Li metal to form LiF layer, restraining the Li dendrite growth. Meanwhile, the polyacrylonitrile (PAN) antioxidant layer strengthens the contact stability between the electrolytes and the cathodes. Moreover, the PP film serves as the electrolyte's skeleton and connecting layer, enhancing the ion diffusion and mechanical strength of the solid electrolytes. As a result, the Li||CSPE@PP||Li cell is able to stably cycle over 400 h at 0.1 mA cm −2 . The LFP||CSPE@PP||Li solid-state batteries deliver 141.98 mAh g −1 discharge capacity and high retention rate (91.1%) after 100 cycles at 0.1C. This work provides a viable strategy for expanding the application of composite solid polymer electrolyte (CSPE) in lithium metal batteries.
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高影响因子
Batteries-Basel
·
2023
·Vol. 9
·期 9
·471
·
IF 4
Shujian Zhang,Hongmo Zhu,Lanfang Que,Xuning Leng,Lei Zhao,Zhenbo Wang
To optimize the preparation process of polymer electrolytes by in situ UV curing and improve the performance of polymer electrolytes, we investigated the effect of carrier film phase conversion time on the properties of polymer electrolyte properties in all-solid-state LIBs. We compared several carrier films with phase conversion times of 24 h, 32 h, 40 h, and 48 h. Then, the physical properties of the polymer electrolytes were characterized and the properties of the polymer electrolytes were further explored. It was concluded that the carrier membrane with a phase transition time of 40 h and the prepared electrolyte had the best performance. The ionic conductivity of the sample was 1.02 × 10−3S/cm at 25 °C and 3.42 × 10−3S/cm at 60 °C. At its best cycle performance, it had the highest discharge-specific capacity of 155.6 mAh/g, and after 70 cycles, the discharge-specific capacity was 152.4 mAh/g, with a capacity retention rate of 98% and a discharge efficiency close to 100%. At the same time, the thermogravimetric curves showed that the samples prepared by this process had good thermal stability which can meet the various requirements of lithium-ion batteries.Keywords:phase conversion time;UV curing;solid polymer electrolyte;porous carrier membrane;lithium-ion battery
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高影响因子
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