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Lithiophilic Li-Si alloy-solid electrolyte interface enabled by high-concentration dual salt-reinforced quasi-solid-state electrolyte
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作者 Yuanxing Zhang Ling Zhang +7 位作者 Zhiguang Zhao Yuxiang Zhang Jingwen Cui Chengcai Liu Daobin Mu Yuefeng Su Borong Wu Feng Wu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第8期216-230,I0005,共16页
Solid polymer electrolytes(SPEs)are urgently required to achieve practical solid-state lithium metal batteries(LMBs)and lithium-ion batteries(LIBs),Herein,we proposed a mechanism for modulating interfacial conduction ... Solid polymer electrolytes(SPEs)are urgently required to achieve practical solid-state lithium metal batteries(LMBs)and lithium-ion batteries(LIBs),Herein,we proposed a mechanism for modulating interfacial conduction and anode interfaces in high-concentration SPEs by LiDFBOP.Optimized electrolyte exhibits superior ionic conductivity and remarkable interface compatibility with salt-rich clusters:(1)polymer-plastic crystal electrolyte(P-PCE,TPU-SN matrix)dissociates ion pairs to facilitate Li+transport in the electrolyte and regulates Li^(+)diffusion in the SEI.The crosslinking structure of the matrix compensates for the loss of mechanical strength at high-salt concentrations;(2)dual-anion TFSI^(-)_(n)-DFBOP^(-)_(m)in the Li^(+)solvation sheath facilitates facile Li^(+)desolvation and formation of salt-rich clusters and is conducive to the formation of Li conductive segments of TPU-SN matrix;(3)theoretical calculations indicate that the decomposition products of LiDFBOP form SEI with lower binding energy with LiF in the SN system,thereby enhancing the interfacial electrochemical redox kinetics of SPE and creating a solid interface SEI layer rich in LiF.As a result,the optimized electrolyte exhibits an excellent ionic conductivity of9.31×10^(-4)S cm^(-1)at 30℃and a broadened electrochemical stability up to 4.73 V.The designed electrolyte effectively prevents the formation of Li dendrites in Li symmetric cells for over 6500 h at0.1 mA cm^(-2).The specific Li-Si alloy-solid state half-cell capacity shows 711.6 mAh g^(-1)after 60 cycles at 0.3 A g^(-1).Excellent rate performance and cycling stability are achieved for these solid-state batteries with Li-Si alloy anodes and NCM 811 cathodes.NCM 811‖Prelithiated silicon-based anode solid-state cell delivers a discharge capacity of 195.55 mAh g^(-1)and a capacity retention of 97.8%after 120 cycles.NCM 811‖Li solid-state cell also delivers capacity retention of 84.2%after 450 cycles. 展开更多
关键词 Prelithiation Li-Si alloy anode Solid-state electrolyte SEI layer
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MOF-based quasi-solid-state electrolyte for long-life Al-Se battery 被引量:1
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作者 Haiping Lei Jiguo Tu +4 位作者 Suqin Li Jiacheng Wang Zheng Huang Zhijing Yu Shuqiang Jiao 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第11期237-245,I0006,共10页
Aluminum-selenium(Al-Se)batteries,which possess a high theoretical specific capacity of 1357 mA h g^(-1),represent a promising energy storage technology.However,they suffer from significant attenuation of capacity and... Aluminum-selenium(Al-Se)batteries,which possess a high theoretical specific capacity of 1357 mA h g^(-1),represent a promising energy storage technology.However,they suffer from significant attenuation of capacity and low cycle life due to the shuttle effect.To mitigate the shuttle effect induced by soluble selenium chloroaluminate compound that tends to migrate towards the negative electrode,a quasi-solid-state Al-Se battery was fabricated through the synthesis of a multi-aperture structure quasisolid-state electrolyte(MOF@GPE)based on metal-organic framework(MOF)material and gel-polymer electrolyte(GPE).The high ionic conductivity(1.13×10^(-3)S cm^(-1))of MOF@GPE at room temperature,coupled with its wide electrochemical stability window(2.45 V),can facilitate ion transport kinetics and enhance the electrochemical performance of Al-Se batteries.The MOF@GPE-based quasi-solidstate Al-Se batteries exhibit outstanding long-life cycling stability,delivering a high specific discharge capacity of 548 mA h g^(-1)with a maintained discharge specific capacity of 345 mA h g^(-1)after 500 cycles at a current density of 200 mA g^(-1).The stable ion transmission and high ion transport kinetics in MOF@GPE can be attributed to the stable structure and permeable channel of MOF,which effectively captures the soluble selenium chloroaluminate compound and further restrains the shuttle effect,resulting in improved cycling performance. 展开更多
关键词 Aluminum selenium batteries MOF quasi-solid-state electrolyte Shuttle effect Transport kinetics
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Deep dive into anionic metal-organic frameworks based quasi-solid-state electrolytes
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作者 Tingzheng Hou Wentao Xu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第6期313-320,I0008,共9页
The development and application of high-capacity energy storage has been crucial to the global transition from fossil fuels to green energy.In this context,metal-organic frameworks(MOFs),with their unique 3D porous st... The development and application of high-capacity energy storage has been crucial to the global transition from fossil fuels to green energy.In this context,metal-organic frameworks(MOFs),with their unique 3D porous structure and tunable chemical functionality,have shown enormous potential as energy storage materials for accommodating or transporting electrochemically active ions.In this perspective,we specifically focus on the current status and prospects of anionic MOF-based quasi-solid-state-electrolytes(anionic MOF-QSSEs)for lithium metal batteries(LMBs).An overview of the definition,design,and properties of anionic MOF-QSSEs is provided,including recent advances in the understanding of their ion transport mechanism.To illustrate the advantages of using anionic MOF-QSSEs as electrolytes for LMBs,a thorough comparison between anionic MOF-QSSEs and other well-studied electrolyte systems is made.With these in-depth understandings,viable techniques for tuning the chemical and topological properties of anionic MOF-QSSEs to increase Li+conductivity are discussed.Beyond modulation of the MOFs matrix,we envisage that solvent and solid-electrolyte interphase design as well as emerging fabrication techniques will aid in the design and practical application of anionic MOF-QSSEs. 展开更多
关键词 Anionic metal–organic frameworks quasi-solid-state electrolytes Ionic conduction Lithium metal batteries Lithium-ion batteries
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Recent advances on quasi-solid-state electrolytes for supercapacitors 被引量:3
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作者 Murilo M.Amaral Raissa Venâncio +1 位作者 Alfredo C.Peterlevitz Hudson Zanin 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第4期697-717,共21页
Solid-state and quasi-solid-state electrolytes have been attracting the scientific community’s attention in the last decade. These electrolytes provide significant advantages, such as the absence of leakage and separ... Solid-state and quasi-solid-state electrolytes have been attracting the scientific community’s attention in the last decade. These electrolytes provide significant advantages, such as the absence of leakage and separators for devices and safety for users. They also allow the assembly of stretchable and bendable supercapacitors. Comparing solid-state to quasi-solid-states, the last provides the most significant energy and power densities due to the better ionic conductivity. Our goal here is to present recent advances on quasisolid-state electrolytes, including gel-polymer electrolytes. We reviewed the most recent literature on quasi-solid-state electrolytes with different solvents for supercapacitors. Organic quasi-solid-state electrolytes need greater attention once they reach an excellent working voltage window greater than 2.5 V.Meanwhile, aqueous-based solid-state electrolytes have a restricted voltage window to less than 2 V. On the other hand, they are easier to handle, provide greater ionic conductivity and capacitance. Recent water-in-salt polymer-electrolytes have shown stability as great as 2 V encouraging further development in aqueous-based quasi-solid-state electrolytes. Moreover, hydrophilic conductive polymers have great commercial appeal for bendable devices. Thus, these electrolytes can be employed in flexible and bendable devices, favoring the improvement of portable electronics and wearable devices(376 references were evaluated and summarized here). 展开更多
关键词 quasi-solid-state electrolyte Gel-polymer electrolyte Flexible supercapacitor Wearables
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A high-performance rechargeable Li–O_2 battery with quasi-solid-state electrolyte
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作者 Jia-Yue Peng Jie Huang +5 位作者 Wen-Jun Li Yi Wang Xiqian Yu Yongsheng Hu Liquan Chen Hong Li 《Chinese Physics B》 SCIE EI CAS CSCD 2018年第7期556-560,共5页
A novel transparent and soft quasi-solid-state electrolyte (QSSE) was proposed and fabricated, which consists of ionic liquid (PYR14TFSI) and nano-fumed silica. The QSSE demonstrates high ionic conductivity of 4.6... A novel transparent and soft quasi-solid-state electrolyte (QSSE) was proposed and fabricated, which consists of ionic liquid (PYR14TFSI) and nano-fumed silica. The QSSE demonstrates high ionic conductivity of 4.6× 10-4 S/cm at room temperature and wide electrochemical stability window of over 5 V. The Li-O2 battery using such quasi-solidstate electrolyte exhibits a low charge-discharge overpotential at the first cycle and excellent long-term cyclability over 500 cycles. 展开更多
关键词 quasi-solid-state electrolyte Li-O2 battery
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Recent research progress on quasi-solid-state electrolytes for dye-sensitized solar cells 被引量:1
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作者 Asif Mahmood 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2015年第6期686-692,共7页
Dye-sensitized solar cells (DSSCs) are the most promising, low cost and most extensively investigated solar cells. They are famous for their clean and efficient solar energy conversion. Nevertheless this, long-time ... Dye-sensitized solar cells (DSSCs) are the most promising, low cost and most extensively investigated solar cells. They are famous for their clean and efficient solar energy conversion. Nevertheless this, long-time sta- bility is still to be acquired. In recent years research on solid and quasi-solid state electrolytes is extensively in- creased. Various quasi-solid electrolytes, including composites polymer electrolytes, ionic liquid electrolytes, thermoplastic polymer electrolytes and thermosetting polymer electrolytes have been used. Performance and stability of a quasi-solid state electrolyte are between liquid and solid electrolytes. High photovoltaic performances of QS-DSSCs along better long-term stability can be obtained by designing and optimizing quasi-solid electrolytes. It is a prospective candidate for highly efficient and stable DSSCs. 展开更多
关键词 Dye-sensitized solar cells Quasi-solid electrolytes Composites polymer electrolytes Ionic liquid electrolytes Thermoplastic polymer electrolytes and thermosetting polymer electrolytes
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Extremely stable Li-metal battery enabled by piezoelectric polyacrylonitrile quasi-solid-state electrolytes 被引量:1
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作者 Hongzhi Peng Zhong Xu +9 位作者 Yunjie Zhou Junfeng Huang Tao Yang Jieling Zhang Yong Ao Yanting Xie Hanyu He Xiong Zhang Weiqing Yang Haitao Zhang 《Journal of Materiomics》 SCIE CSCD 2024年第1期134-144,共11页
Polymer solid-state electrolytes(PSSEs)are promising for solving the safety problem of Lithium(Li)metal batteries(LMBs).However,PSSEs with low modulus in nature are prone to be penetrated by lithium dendrites,resultin... Polymer solid-state electrolytes(PSSEs)are promising for solving the safety problem of Lithium(Li)metal batteries(LMBs).However,PSSEs with low modulus in nature are prone to be penetrated by lithium dendrites,resulting in short circuit of LMBs.Here,we design and prepare piezoelectric BaTiO_(3)doped polyacrylonitrile(PAN@BTO)quasi-solid-state electrolytes(PQSSEs)by electrostatic spinning method to suppress dendritic growth.The piezoelectric polymer electrolytes are squeezed by nucleation and growth processes of Li dendrites,which can generate a piezoelectric electric field to regulate the deposition of Li^(+)ions and eliminate lithium bud.Consequently,piezoelectric PAN@BTO PQSSEs enables highly stable Li plating/stripping cycling for over 2000 h at 0.15 mA/cm^(2)at room temperature(RT,25℃).Also,LiFePO_(4)|PAN@BTO|Li full cells demonstrate excellent cycle performance(136.9 mA·h/g and 78%retention after 600 cycles at 0.5 C)at RT.Moreover,LiFePO_(4)|PAN@BTO|Li battery show extremely high safety and can still work normally under high-speed impact(2 Hz,∼30 kPa).We construct an in-situ cell monitoring system and disclose that the mechanism of suppressed lithium dendrite is originated from the generation of opposite piezoelectric potential and the feedback speed of intermittent piezoelectric potential signals is extremely fast. 展开更多
关键词 Polymer solid-state electrolytes POLYACRYLONITRILE Piezoelectric effect Lithium metal battery Long-term stability Lithium dendrites
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Dual-salt poly(tetrahydrofuran) electrolyte enables quasi-solid-state lithium metal batteries to operate at -30 ℃
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作者 Zhiyong Li Zhuo Li +1 位作者 Rui Yu Xin Guo 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第9期456-463,共8页
The stable operation of solid-state lithium metal batteries at low temperatures is plagued by severe restrictions from inferior electrolyte-electrode interface compatibility and increased energy barrier for Li^(+)migr... The stable operation of solid-state lithium metal batteries at low temperatures is plagued by severe restrictions from inferior electrolyte-electrode interface compatibility and increased energy barrier for Li^(+)migration.Herein,we prepare a dual-salt poly(tetrahydrofuran)-based electrolyte consisting of lithium hexafluorophosphate and lithium difluoro(oxalato)borate(LiDFOB).The Li-salt anions(DFOB−)not only accelerate the ring-opening polymerization of tetrahydrofuran,but also promote the formation of highly ion-conductive and sustainable interphases on Li metal anodes without sacrificing the Li^(+)conductivity of electrolytes,which is favorable for Li^(+)transport kinetics at low temperatures.Applications of this polymer electrolyte in Li||LiFePO_(4)cells show 82.3%capacity retention over 1000 cycles at 30℃and endow stable discharge capacity at−30℃.Remarkably,the Li||LiFePO4 cells retain 52%of their room-temperature capacity at−20℃and 0.1 C.This rational design of dual-salt polymer-based electrolytes may provide a new perspective for the stable operation of quasi-solid-state batteries at low temperatures. 展开更多
关键词 Poly(tetrahydrofuran) Dual-salt electrolyte Solidel ectrolyte interphase Low-temperature operation quasi-solid-state battery
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A"Concentrated lonogel-in-Ceramic"Silanization Composite Electrolyte with Superior Bulk Conductivity and Low Interfacial Resistance for Quasi-Solid-State Li Metal Batteries
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作者 Wangshu Hou Zongyuan Chen +4 位作者 Shengxian Wang Fengkun Wei Yanfang Zhai Ning Hu Shufeng Song 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第5期20-28,共9页
The ideal composite electrolyte for the pursued safe and high-energy-density lithium metal batteries(LMBs)is expected to demonstrate peculiarity of superior bulk conductivity,low interfacial resistances,and good compa... The ideal composite electrolyte for the pursued safe and high-energy-density lithium metal batteries(LMBs)is expected to demonstrate peculiarity of superior bulk conductivity,low interfacial resistances,and good compatibility against both Li-metal anode and high-voltage cathode.There is no composite electrolyte to synchronously meet all these requirements yet,and the battery performance is inhibited by the absence of effective electrolyte design.Here we report a unique"concentrated ionogel-in-ceramic"silanization composite electrolyte(SCE)and validate an electrolyte design strategy based on the coupling of high-content silane-conditioning garnet and concentrated ionogel that builds well-percolated Li+transport pathways and tackles the interface issues to respond all the aforementioned requirements.It is revealed that the silane conditioning enables the uniform dispersion of garnet nanoparticles at high content(70 wt%)and forms mixed-lithiophobic-conductive LiF-Li3N solid electrolyte interphase.Notably,the yielding SCE delivers an ultrahigh ionic conductivity of 1.76 X 10^(-3)S cm^(-1)at 25℃,an extremely low Li-metal/electrolyte interfacial area-specific resistance of 13Ωcm^(2),and a distinctly excellent long-term 1200 cycling without any capacity decay in 4.3 V Li‖LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2)(NCM523)quasi-solid-state LMB.This composite electrolyte design strategy can be extended to other quasi-/solid-state LMBs. 展开更多
关键词 composite electrolyte concentrated ionogel-in-ceramic interfacial resistance SILANE solid electrolyte interphase
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Stretchable alkaline quasi-solid-state electrolytes created by super-tough, fatigue-resistant and alkali-resistant multi-bond network hydrogels
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作者 Hao Xu Yujun Liu Xu-Ming Xie 《Chinese Chemical Letters》 SCIE CAS CSCD 2023年第4期275-278,共4页
Hydrogel-based quasi-solid-state electrolytes(Q-SSEs) swollen with electrolyte solutions are important components in stretchable supercapacitors and other wearable devices. This work fabricates a supertough, fatigue-r... Hydrogel-based quasi-solid-state electrolytes(Q-SSEs) swollen with electrolyte solutions are important components in stretchable supercapacitors and other wearable devices. This work fabricates a supertough, fatigue-resistant, and alkali-resistant multi-bond network(MBN) hydrogel aiming to be an alkaline Q-SSE. To synthesize the hydrogel, a 2-ureido-4[1H]-pyrimidone(UPy) motif is introduced into a poly(acrylic acid) polymer chain. The obtained MBN hydrogels with 75 wt% water content exhibit tensile strength as high as 2.47 MPa, which is enabled by the large energy dissipation ability originated from the dissociation of UPy dimers due to their high bond association energy. Owing to the high dimerization constant of UPy motifs, the dissociated UPy motifs are able to partially re-associate soon after being released from external forces, resulting in excellent fatigue-resistance. More importantly, the MBN hydrogels exhibit excellent alkali-resistance ability. The UPy Gel-10 swollen with 1 mol/L KOH display a tensile strength as high as ~1.0 MPa with elongation at break of ~550%. At the same time, they show ionic conductivity of ~17 m S/cm, which do not decline even when the hydrogels are stretched to 500% strain.The excellent mechanical property and ionic conductivity of the present hydrogels demonstrate potential application as a stretchable alkaline Q-SSE. 展开更多
关键词 Alkaline quasi-solid-state electrolyte Super-tough hydrogel Fatigue resistance Alkali resistance Multi-bond network
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COF-based single Li^(+)solid electrolyte accelerates the ion diffusionandrestrains dendritegrowthin quasi-solid-state organic batteries 被引量:3
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作者 Genfu Zhao Zhiyuan Mei +5 位作者 Lingyan Duan Qi An Yongxin Yang Conghui Zhang Xiaoping Tan Hong Guo 《Carbon Energy》 SCIE CSCD 2023年第2期171-183,共13页
A solid-state electrolyte(SSE),which is a solid ionic conductor and electroninsulating material,is known to play a crucial role in adapting a lithium metal anode to a high-capacity cathode in a solid-state battery.Amo... A solid-state electrolyte(SSE),which is a solid ionic conductor and electroninsulating material,is known to play a crucial role in adapting a lithium metal anode to a high-capacity cathode in a solid-state battery.Among the various SSEs,the single Li-ion conductor has advantages in terms of enhancing the ion conductivity,eliminating interfacial side reactions,and broadening the electrochemical window.Covalent organic frameworks(COFs)are optimal platforms for achieving single Li-ion conduction behavior because of wellordered one-dimensional channels and precise chemical modification features.Herein,we study in depth three types of Li-carboxylate COFs(denoted LiOOC-COFn,n=1,2,and 3)as single Li-ion conducting SSEs.Benefiting from well-ordered directional ion channels,the single Li-ion conductor LiOOC-COF3 shows an exceptional ion conductivity of 1.36×10^(-5) S cm^(-1) at room temperature and a high transference number of 0.91.Moreover,it shows excellent electrochemical performance with long-term cycling,high-capacity output,and no dendrites in the quasi-solid-state organic battery,with the organic small molecule cyclohexanehexone(C_(6)O_(6))as the cathode and the Li metal as the anode,and enables effectively avoiding dissolution of the organic electrode by the liquid electrolyte. 展开更多
关键词 covalent organic frameworks quasi-solid-state organic battery single Li-ion conductor solid-state electrolyte
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Molecular Reactivity and Interface Stability Modification in In-Situ Gel Electrolyte for High Performance Quasi-Solid-State Lithium Metal Batteries 被引量:2
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作者 Qiyu Wang Xiangqun Xu +4 位作者 Bo Hong Maohui Bai Jie Li Zhian Zhang Yanqing Lai 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2023年第3期8-19,共12页
Quasi-solid-state lithium metal battery is a promising candidate for next generation high energy density and high safety power supply.Despite intensive efforts on electrolytes,uncontrolled interfacial reactions on lit... Quasi-solid-state lithium metal battery is a promising candidate for next generation high energy density and high safety power supply.Despite intensive efforts on electrolytes,uncontrolled interfacial reactions on lithium with electrolyte and patchy interfacial contacts still hinder its practical process.Herein,we bring in rationally designed F contained groups into polymer skeleton via in-situ gelation for the first time to establish quasi-solid-state battery.This method achieves a capacity retention of 90%after 1000 cycles at 0.5C with LiFePO_(4)cathodes.The interface constructed by polymer skeleton and reaction with–CF_(3)lead to the predicted solid electrolyte interface species with high stability.Furthermore,we optimize molecular reactivity and interface stability with regulating F contained end groups in the polymer.Comparisons on different structures reveal that high performance solid stable lithium metal batteries rely on chemical modification as well as stable polymer skeleton,which is more critical to construct robust and steady SEI with uniform lithium deposition.New approach with functional groups regulation proposes a more stable cycling process with a capacity retention of 94.2%at 0.5C and 87.6%at 1C after 1000 cycles with LiFePO_(4) cathodes,providing new insights for the practical development of quasi-solid-state lithium metal battery. 展开更多
关键词 F contained end groups in-situ gel electrolyte interface stability molecular reactivity quasi-solid-state lithium metal battery
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A UV cross-linked gel polymer electrolyte enabling high-rate and high voltage window for quasi-solid-state supercapacitors 被引量:1
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作者 Yuge Bai Chao Yang +6 位作者 Boheng Yuan Hongjie Li Weimeng Chen Haosen Yin Bin Zhao Fei Shen Xiaogang Han 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第1期41-50,I0002,共11页
Serving as a promising alternative to liquid electrolyte in the application of portable and wearable devices,gel polymer electrolytes(GPEs)are expected to obtain more preferable properties rather than just be satisfie... Serving as a promising alternative to liquid electrolyte in the application of portable and wearable devices,gel polymer electrolytes(GPEs)are expected to obtain more preferable properties rather than just be satisfied with the merits of high safety and deformability.Here,an easy-operated method is employed to fabricate cross-linked composite polymer membranes used for GPEs assisted by UV irradiation,in which N-doped carbon quantum dots(N-CQDs)and TiO2are introduced as photocatalysts and additives to improve the performances of GPEs.Specifically,N-CQDs participate as a cross-linker to construct the inner porous structure,and TiO2nanoparticles serve as a stabilizer to improve the electrochemical stability of GPEs under high voltage(3.5 V).The excellent thermal and mechanical stability of the membrane fabricated in this work guarantee the safety of the supercapacitors(SCs).This GPE based SC not only exhibits prominent rate performance(105%capacitance retention at the current density of 40A g^(-1))and cyclic stability(85%at 1 A g^(-1)under 3.5 V after 20,000 cycles),but also displays remarkable energy density(42.88 Wh kg^(-1))with high power density(19.3 k W kg^(-1)).Moreover,the superior rate and cycling performances of the as-prepared GPE based flexible SCs under flat and bending state confirm the feasibility of its application in flexible energy storage devices. 展开更多
关键词 Gel polymer electrolyte UV cross-linking Energy density High voltage window
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High-Performance Quasi-Solid-State Pouch Cells Enabled by in situ Solidification of a Novel Polymer Electrolyte 被引量:3
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作者 Qingwen Lu Changhong Wang +9 位作者 Danni Bao Hui Duan Feipeng Zhao Kieran Doyle-Davis Qiang Zhang Rennian Wang Shangqian Zhao Jiantao Wang Huan Huang Xueliang Sun 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2023年第4期15-21,共7页
Conventional lithium-ion batteries(LIBs)with liquid electrolytes are challenged by their big safety concerns,particularly used in electric vehicles.All-solid-state batteries using solid-state electrolytes have been pr... Conventional lithium-ion batteries(LIBs)with liquid electrolytes are challenged by their big safety concerns,particularly used in electric vehicles.All-solid-state batteries using solid-state electrolytes have been proposed to significantly improve safety yet are impeded by poor interfacial solid–solid contact and fast interface degradation.As a compromising strategy,in situ solidification has been proposed in recent years to fabricate quasi-solid-state batteries,which have great advantages in constructing intimate interfaces and cost-effective mass manufacturing.In this work,quasi-solid-state pouch cells with high loading electrodes(≥3 m Ah cm^(-2))were fabricated via in situ solidification of poly(ethylene glycol)diacrylate-based polymer electrolytes(PEGDA-PEs).Both single-layer and multilayer quasi-solid-state pouch cells(2.0 Ah)have demonstrated stable electrochemical performance over500 cycles.The superb electrochemical stability is closely related to the formation of robust and compatible interphase,which successfully inhibits interfacial side reactions and prevents interfacial structural degradation.This work demonstrates that in situ solidification is a facile and cost-effective approach to fabricate quasi-solid-state pouch cells with both excellent electrochemical performance and safety. 展开更多
关键词 high areal capacity high-energy-density pouch cells in situ solidification poly(ethylene glycol)diacrylate-based polymer electrolyte
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Porous Organic Cage‑Based Quasi‑Solid‑State Electrolyte with Cavity‑Induced Anion‑Trapping Effect for Long‑Life Lithium Metal Batteries
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作者 Wei-Min Qin Zhongliang Li +7 位作者 Wen‑Xia Su Jia‑Min Hu Hanqin Zou Zhixuan Wu Zhiqin Ruan Yue‑Peng Cai Kang Li Qifeng Zheng 《Nano-Micro Letters》 SCIE EI CAS 2025年第2期376-386,共11页
Porous organic cages(POCs)with permanent porosity and excellent host–guest property hold great potentials in regulating ion transport behavior,yet their feasibility as solid-state electrolytes has never been testifie... Porous organic cages(POCs)with permanent porosity and excellent host–guest property hold great potentials in regulating ion transport behavior,yet their feasibility as solid-state electrolytes has never been testified in a practical battery.Herein,we design and fabricate a quasi-solid-state electrolyte(QSSE)based on a POC to enable the stable operation of Li-metal batteries(LMBs).Benefiting from the ordered channels and cavity-induced anion-trapping effect of POC,the resulting POC-based QSSE exhibits a high Li+transference number of 0.67 and a high ionic conductivity of 1.25×10^(−4) S cm^(−1) with a low activation energy of 0.17 eV.These allow for homogeneous Li deposition and highly reversible Li plating/stripping for over 2000 h.As a proof of concept,the LMB assembled with POC-based QSSE demonstrates extremely stable cycling performance with 85%capacity retention after 1000 cycles.Therefore,our work demonstrates the practical applicability of POC as SSEs for LMBs and could be extended to other energy-storage systems,such as Na and K batteries. 展开更多
关键词 Porous organic cage Cavity-induced anion-trapping quasi-solid-state electrolyte Homogeneous Li+flux Lithium metal battery
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A quasi-solid-state electrolyte with high ionic conductivity for stable lithium-ion batteries 被引量:3
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作者 ZHANG WenJing LI SenLin +3 位作者 ZHANG YuRong WANG XingHui LIU JingDong ZHENG YuanHui 《Science China(Technological Sciences)》 SCIE EI CAS CSCD 2022年第10期2369-2379,共11页
The practical applications of solid-state electrolytes in lithium-ion batteries(LIBs)are hindered by their low ionic conductivity and high interfacial resistance.Herein,an ethoxylated trimethylolpropane triacrylate ba... The practical applications of solid-state electrolytes in lithium-ion batteries(LIBs)are hindered by their low ionic conductivity and high interfacial resistance.Herein,an ethoxylated trimethylolpropane triacrylate based quasi-solid-state electrolyte(ETPTAQSSE)with a three-dimensional(3D)network is prepared by a one-step in-situ photopolymerization method.The 3D network is designed to overcome the contradiction between the plasticizer-related ionic conductivity and the thickness-dependent mechanical property of quasi-solid-state electrolytes.The ETPTA-QSSE achieves superb room-temperature ionic conductivity up to 4.55×10^(−3)S cm^(−1),a high lithium ion transference number of 0.57,along with a wide electrochemical window of 5.3 V(vs.Li+/Li),which outperforms most ever of the reported solid-state electrolytes.Owing to the robust network structure and the cathodeelectrolyte integrated electrode design,Li metal symmetrical cells show reduced interface resistance and reinforced electrode/electrolyte interface stability.When applying the ETPTA-QSSE in LiFePO_(4)||Li cells,the quasi-solid-state cell demonstrates an enhanced initial discharge capacity(155.5 mAh g^(−1)at 0.2 C)accompanied by a high average Coulombic efficiency of greater than 99.3%,offering capacity retention of 92%after 200 cycles.Accordingly,this work sheds light on the strategy of enhancing ionic conductivity and reducing interfacial resistance of quasi-solid-state electrolytes,which is promising for high-voltage LIBs. 展开更多
关键词 quasi-solid-state electrolyte ionic conductivity electrochemical window PHOTOPOLYMERIZATION lithium-ion batteries
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Unique double-layer solid electrolyte interphase formed with fluorinated ether-based electrolytes for high-voltage lithium metal batteries 被引量:2
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作者 Ruo Wang Jiawei Li +11 位作者 Bing Han Qingrong Wang Ruohong Ke Tong Zhang Xiaohu Ao Guangzhao Zhang Zhongbo Liu Yunxian Qian Fangfang Pan Iseult Lynch Jun Wang Yonghong Deng 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第1期532-542,I0012,共12页
Li metal batteries using high-voltage layered oxides cathodes are of particular interest due to their high energy density.However,they suffer from short lifespan and extreme safety concerns,which are attributed to the... Li metal batteries using high-voltage layered oxides cathodes are of particular interest due to their high energy density.However,they suffer from short lifespan and extreme safety concerns,which are attributed to the degradation of layered oxides and the decomposition of electrolyte at high voltage,as well as the high reactivity of metallic Li.The key is the development of stable electrolytes against both highvoltage cathodes and Li with the formation of robust interphase films on the surfaces.Herein,we report a highly fluorinated ether,1,1,1-trifluoro-2-[(2,2,2-trifluoroethoxy)methoxy]ethane(TTME),as a cosolvent,which not only functions as a diluent forming a localized high concentration electrolyte(LHCE),but also participates in the construction of the inner solvation structure.The TTME-based electrolyte is stable itself at high voltage and induces the formation of a unique double-layer solid electrolyte interphase(SEI)film,which is embodied as one layer rich in crystalline structural components for enhanced mechanical strength and another amorphous layer with a higher concentration of organic components for enhanced flexibility.The Li||Cu cells display a noticeably high Coulombic efficiency of 99.28%after 300 cycles and Li symmetric cells maintain stable cycling more than 3200 h at 0.5 mA/cm^(2) and 1.0m Ah/cm^(2).In addition,lithium metal cells using LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) and Li CoO_(2) cathodes(both loadings~3.0 m Ah/cm^(2))realize capacity retentions of>85%over 240 cycles with a charge cut-off voltage of 4.4 V and 90%for 170 cycles with a charge cut-off voltage of 4.5 V,respectively.This study offers a bifunctional ether-based electrolyte solvent beneficial for high-voltage Li metal batteries. 展开更多
关键词 Lithium metal batteries High-voltage layered oxides Fluorinated ether-based electrolytes Solid electrolyte interphase Cathode electrolyte interphase
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Trend of Developing Aqueous Liquid and Gel Electrolytes for Sustainable,Safe,and High‑Performance Li‑Ion Batteries 被引量:2
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作者 Donghwan Ji Jaeyun Kim 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第1期17-34,共18页
Current lithium-ion batteries(LIBs)rely on organic liquid electrolytes that pose significant risks due to their flammability and toxicity.The potential for environmental pollution and explosions resulting from battery... Current lithium-ion batteries(LIBs)rely on organic liquid electrolytes that pose significant risks due to their flammability and toxicity.The potential for environmental pollution and explosions resulting from battery damage or fracture is a critical concern.Water-based(aqueous)electrolytes have been receiving attention as an alternative to organic electrolytes.However,a narrow electrochemicalstability window,water decomposition,and the consequent low battery operating voltage and energy density hinder the practical use of aqueous electrolytes.Therefore,developing novel aqueous electrolytes for sustainable,safe,high-performance LIBs remains challenging.This Review first commences by summarizing the roles and requirements of electrolytes–separators and then delineates the progression of aqueous electrolytes for LIBs,encompassing aqueous liquid and gel electrolyte development trends along with detailed principles of the electrolytes.These aqueous electrolytes are progressed based on strategies using superconcentrated salts,concentrated diluents,polymer additives,polymer networks,and artificial passivation layers,which are used for suppressing water decomposition and widening the electrochemical stability window of water of the electrolytes.In addition,this Review discusses potential strategies for the implementation of aqueous Li-metal batteries with improved electrolyte–electrode interfaces.A comprehensive understanding of each strategy in the aqueous system will assist in the design of an aqueous electrolyte and the development of sustainable and safe high-performance batteries. 展开更多
关键词 Lithium-ion battery(LIB) Aqueous electrolyte Gel electrolyte Electrochemical stability window Li dendrite
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Challenges in Li-ion battery high-voltage technology and recent advances in high-voltage electrolytes 被引量:1
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作者 Jianguo Liu Baohui Li +2 位作者 Jinghang Cao Xiao Xing Gan Cui 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第4期73-98,共26页
The electrolyte directly contacts the essential parts of a lithium-ion battery,and as a result,the electrochemical properties of the electrolyte have a significant impact on the voltage platform,charge discharge capac... The electrolyte directly contacts the essential parts of a lithium-ion battery,and as a result,the electrochemical properties of the electrolyte have a significant impact on the voltage platform,charge discharge capacity,energy density,service life,and rate discharge performance.By raising the voltage at the charge/discharge plateau,the energy density of the battery is increased.However,this causes transition metal dissolution,irreversible phase changes of the cathode active material,and parasitic electrolyte oxidation reactions.This article presents an overview of these concerns to provide a clear explanation of the issues involved in the development of electrolytes for high-voltage lithium-ion batteries.Additionally,solidstate electrolytes enable various applications and will likely have an impact on the development of batteries with high energy densities.It is necessary to improve the high-voltage performance of electrolytes by creating solvents with high thermal stabilities and high voltage resistance and additives with superior film forming performance,multifunctional capabilities,and stable lithium salts.To offer suggestions for the future development of high-energy lithium-ion batteries,we conclude by offering our own opinions and insights on the current development of lithium-ion batteries. 展开更多
关键词 Lithium-ion battery High voltage electrolyte additive Solid electrolyte
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Electrolyte Design for Low‑Temperature Li‑Metal Batteries:Challenges and Prospects 被引量:1
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作者 Siyu Sun Kehan Wang +3 位作者 Zhanglian Hong Mingjia Zhi Kai Zhang Jijian Xu 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第2期365-382,共18页
Electrolyte design holds the greatest opportunity for the development of batteries that are capable of sub-zero temperature operation.To get the most energy storage out of the battery at low temperatures,improvements ... Electrolyte design holds the greatest opportunity for the development of batteries that are capable of sub-zero temperature operation.To get the most energy storage out of the battery at low temperatures,improvements in electrolyte chemistry need to be coupled with optimized electrode materials and tailored electrolyte/electrode interphases.Herein,this review critically outlines electrolytes’limiting factors,including reduced ionic conductivity,large de-solvation energy,sluggish charge transfer,and slow Li-ion transportation across the electrolyte/electrode interphases,which affect the low-temperature performance of Li-metal batteries.Detailed theoretical derivations that explain the explicit influence of temperature on battery performance are presented to deepen understanding.Emerging improvement strategies from the aspects of electrolyte design and electrolyte/electrode interphase engineering are summarized and rigorously compared.Perspectives on future research are proposed to guide the ongoing exploration for better low-temperature Li-metal batteries. 展开更多
关键词 Solid electrolyte interphase Li metal Low temperature electrolyte design BATTERIES
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