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A quasi-solid-state electrolyte with high ionic conductivity for stable lithium-ion batteries

Science China(Technological Sciences) 2022年第10期65卷 2369-2379页

作者： ZHANG WenJing LI SenLin ZHANG YuRong WANG XingHui LIU JingDong ZHENG YuanHui College of Chemistry Fujian Provincial Key Laboratory of Advanced Inorganic Oxygenated MaterialsFuzhou UniversityFuzhou 350108China College of Physics and Information Engineering Fuzhou UniversityFuzhou 350108China

The practical applications of solid-state electrolytes in lithium-ion batteries(LIBs)are hindered by their low ionic conductivity and high interfacial ***,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 *** 3D network is designed to overcome the contradiction between the plasticizer-related ionic conductivity and the thickness-dependent mechanical property of quasi-solid-state *** 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(***+/Li),which outperforms most ever of the reported solid-state *** to the robust network structure and the cathodeelectrolyte integrated electrode design,Li metal symmetrical cells show reduced interface resistance and reinforced electrode/electrolyte interface *** 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 ***,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.

关键词： quasi-solid-state electrolyte ionic conductivity electrochemical window photopolymerization lithium-ion batteries

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3D spiny AlF_(3)/Mullite heterostructure nanofiber as solid-state polymer electrolyte fillers with enhanced ionic conductivity and improved interfacial compatibility

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Journal of Energy Chemistry 2023年第1期76卷 503-515,I0013页

作者： Weicui Liu Lingshuai Meng Xueqiang Liu Lu Gao Xiaoxiao Wang Junbao Kang Jingge Ju Nanping Deng Bowen Cheng Weimin Kang State Key Laboratory of Separation Membranes and Membrane Processes/National Center for International Joint Research on Separation Membranes School of Textile Science and Engineering Tiangong UniversityTianjin 300387China Institute of Systems Engineering Beijing 100010Chin

Lithium metal batteries assembled with solid-state electrolyte can offer high safety and volumetric energy density compared to liquid *** polymer solid-state electrolytes of poly(ethylene oxide)(PEO)are widely used in lithium metal solid-state batteries due to their unique ***,there are still some defects such as low ionic conductivity at room temperature and weak inhibition of lithium dendrite ***,the spiny inorganic nanofibers heterostructure with mullite whiskers grown on the surface of aluminum fluoride(AlF_(3))nanofibers are introduced into the PEOLi TFSI electrolytes for the first time to prepare composite solid-state *** AlF_(3)as a strong Lewis acid can adsorb anions and promote the dissociation of Li ***,the specially threedimensional(3D)structure enlarges the effective contacting interface with the PEO polymer,which allows the lithium ions to be transported not only along the large aspect ratio of AlF3nanofibers,but also along the mullite phase in the transmembrane direction ***,the transport channel of lithium ions at the spiny inorganic nanofibers-polymer interface is further *** from these advantages,the obtained composite solid-state electrolyte has a high ionic conductivity of 1.58×10^(-4)S cm^(-1)at 30℃and the lithium ions transfer number of *** addition,the AlF3has strong binding energy with anions,low electronic conductivity and wide electrochemical stability window,and reduced nucleation overpotential of lithium during cycling,which is positive for lithium dendrite suppression in solid-state ***,the assembled symmetric Li/Li symmetric batteries exhibit stable cycling performance at different area capacities of 0.15,0.2,0.3 and 0.4 m A h cm^(-2).More importantly,the LiFePO_(4)(LFP)/Li battery still has 113.5 m A h g-1remaining after 400 cycles at 50℃and the Coulomb efficiency is nearly 100%during the long ***,the interconnected struct

关键词： 3D spiny inorganic nanofibers Heterostructures Composite solid-state electrolytes ionic conductivity

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Rotational motion of polyanion versus volume effect associated with ionic conductivity of several solid electrolytes

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Rare Metals 2018年第6期37卷 497-503页

作者： Qian Zhao Li Pan Yuan-Ji Li Li-Quan Chen Si-Qi Shi Materials Genome Institute Shanghai University School of Materials Science and Engineering Shanghai University Qianweichang College Shanghai University Institute of Physics Chinese Academy of Sciences

Volume effect has been extensively investigated in several families of solid electrolytes, i.e., expanding the skeleton lattice by bigger-size substitution favors the ionic conduction. However, this effect is not applicable in α-Li2SO4 and α-Na3PO4 based inorganic ionic plastic crystal electrolytes, a unique family of solid electrolytes. Here, it is proposed that the underlying rotational motion effect of polyanion, which is actually inhibited by the substitution of bigger-size polyanion in single-phase solid solution region and causes the unexpected lowering of the ionic conductivity instead, should need the more consideration. Furthermore, through utilizing the rotational motion effect of polyanion, it is given that a new explanation of the ionic conductivities of Li10MP2S12 （M = Si, Ge, Se） electrolytes deviating from the volume effect. These results inspire new vision of rationalization of the high-performance solid electrolytes by tuning the rotational motion effect of polyanion.

关键词： Volume effect Rotational motion ofpolyanion ionic conductivity Inorganic plastic crystalelectrolyte

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Increasing ionic conductivity in Li_(0.33)La_(0.56)TiO_(3)thin-films via optimization of processing atmosphere and temperature

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Rare Metals 2022年第1期41卷 179-188页

作者： Shi-Pai Song Cheng Yang Chun-Zhi Jiang Yong-Min Wu Rui Guo He Sun Jing-Lei Yang Yong Xiang Xiao-Kun Zhang School of Materials and Energy University of Electronic Science and Technology of ChinaChengdu 611731China School of Materials Science and Engineering Harbin Institute of TechnologyHarbin 150001China State Key Laboratory of Space Power-Sources Technology Shanghai Institute of Space Power-SourcesShanghai 200245China Department of Mechanical and Aerospace Engineering Hong Kong University of Science and TechnologyHong Kong 999077China Advanced Energy Research Institute University of Electronic Science and Technology of ChinaChengdu 611731China Sichuan Provincial Engineering Research Center of Flexible Display Material Genome University of Electronic Science and Technology of ChinaChengdu 611731China

As a promising solid electrolyte for thin-film lithium batteries,the amorphous Li_(0.33)La_(0.56)TiO_(3)(LLTO)thin film has gained great ***,enhancing ionic conductivity remains challenging in the ***,a systematical study was performed to improve the ionic conductivity of sputter-deposited LLTO thin films via the optimization of processing atmosphere and *** combining the optimized oxygen partial pressure(30%),annealing temperature(300℃),and annealing atmosphere(air),an amorphous LLTO thin film with an ionic conductivity of 5.32910^(-5)·S·cm^(-1) at room temperature and activation energy of 0.26 eV was *** results showed that,first,the oxygen partial pressure should be high enough to compensate for the oxygen loss,but low enough to avoid the abusive oxygen scattering effect on lithium precursors that results in a lithium-poor *** oxygen partial pressure needs to achieve a balance between lithium loss and oxygen defects to improve the ionic ***,a proper annealing temperature reduces the oxygen defects of LLTO thin films while maintaining its amorphous state,which improves the ionic ***,the highest ionic conductivity for the LLTO thin films that were annealed in air(a static space without a gas stream)occurs because of the decreased lithium loss and oxygen defects during *** findings show that the lithium-ion concentration and oxygen defects affect the ionic conductivity for amorphous LLTO thin films,which provides insight into the optimization of LLTO thin-film solid electrolytes,and generates new opportunities for their application in thinfilm lithium batteries.

关键词： Li_(0.33)La_(0.56)TiO_(3) Thin film ionic conductivity Lithium-ion concentration Oxygen defects

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Room-temperature ionic conductivity of Ba,Y,Al co-doped Li_(7)La_(3)Zr_(2)O_(12)solid electrolyte after sintering

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Rare Metals 2021年第8期40卷 2301-2306页

作者： Xiao-Zhen Liu Lei Ding Yu-Ze Liu Li-Ping Xiong Jie Chen Xiao-Long Luo School of Chemical and Environmental Engineering Shanghai Institute of TechnologyShanghai201418China College of Economic and Management Beijing Forestry UniversityBeijing100083China Regenia AB Stockholm10691Sweden

The Ba,Y and A1 co-doped Li_(7)La_(3)Zr_(2)O_(12)(LLZO)was prepared by the solid-state reaction *** of sintering on the crystallographic structure,morphology,total conductivity,relative density and contractibility rate of the prepared solid electrolyte was studied,*** sintered samples were characterized by X-ray diffractometer(XRD),scanning electron microscopy(SEM),electrochemical impedance spectra(EIS)and inductively coupled plasma atomic emission spectrometry(ICP-AES)techniques,*** cubic garnet phase Ba,Y and Al co-doped LLZO is obtained,and the room-temperature total conductivity of the Ba,Y and Al co-doped LLZO solid electrolyte is improved significantly by eliminating the grain boundary resistances and improving the densifications with controlling sintering temperature(T)and time(t),*** at 1160-1190℃for 12 h and at 1190℃for6-15 h,respectively,the Ba,Y and Al co-doped LLZO solid electrolytes are cubic garnet *** at1180-1190℃for 12 h and at 1190℃for 12-18 h,respectively,SEM images of the cross section of the Ba,Y and Al co-doped LLZO solid electrolytes exhibit the distinctively flattened morphology without any noticeable grain *** total conductivity,relative density and contractibility rate of Li_(6.52)La_(2.98)-Ba_(0.02)Zr_(1.9)Y_(0.1)Al_(0.2)O_(12)solid electrolyte are 2.96×10^(-4) S·cm^(-1),94.19%and 18.61%,respectively.

关键词： Solid electrolyte ionic conductivity Sintering Li_(7)La_(3)Zr_(2)O_(12) Garnet

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Preparation of Ultrafine Li4+x AlxSi1-xO4 by Sol-Gel Method and Its ionic conductivity

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Rare Metals 2000年第3期19卷 231-236页

作者： Chen Rufen,Song Xiuqin and Liu Huating (陈汝芬) (宋秀芹) (刘华亭) Department of Chemistry,Hebei Normal University,Shijiazhuang 050016,China 河北师范大学化学系河北石家庄 050016 河北师范大学河北石家庄 050016

Solid electrolyte Li 4+ x Al x Si 1- x O 4 ( x =0～0.5) was prepared by sol gel *** powder samples were characterized by DTA TG,TEM,SEM and XRD. ionic conductivity of the sintered sample was determined by means of A C impedance *** experimental results show that the solid solution range was 0conductivity of samples rised with increasing amount of Al 2O 3 added,the maximum conductivity of Li 4.4 Al 0.4 Si 0.6 O 4 was 8.612×10 -3 S·cm -1 at 300℃.The average grain size of samples was 70 *** sample prepared by sol gel method required lower temperature and presented higher ionic conductivity compared with the samples by the conventional solid state reaction.

关键词： Li 4+ x Al x Si 1- x O 4 Sol Gel method ionic conductivity

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Organic fast ion-conductor with ordered Li-ion conductive nano-pathways and high ionic conductivity for electrochemical energy storage

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Journal of Energy Chemistry 2022年第3期31卷 647-656,I0017页

作者： Yibin Yang He Zhou Jiaying Xie Lixia Bao Tianshi Li Jingxin Lei Jiliang Wang School of Chemical Science and Technology Yunnan UniversityKunming 650091YunnanChina State Key Laboratory of Polymer Materials Engineering Polymer Research Institute of Sichuan UniversityChengdu 610065SichuanChina

Solid electrolyte(SE)is the most crucial factor to fabricate safe and high-performance all-solid-state lithium-ion ***,the most commonly reported SE,including solid polymer electrolyte(SPE)and inorganic oxides and sulfides,suffer problems of low ionic conductivity at room temperature for SPE and large interfacial impedance with electrodes for inorganic *** we for the first time demonstrate a novel ionic plastic crystal lithium salt solid electrolyte(OLiSSE)fast ion-conductor dilithium(1,3-diethyl-4,5-dicarboxylate)imidazole bromide with ordered Li-ion conductive nanopathways and an exceptional ionic conductivity of 4.4×10^(−3)Scm^(−1)at 30℃.The prepared OLiSSE exhibits apparent characters of typical ionic plastic crystals in the temperature range of−20 to 70℃,and shows remarkable thermal stability and electrochemical stability below 150℃ and 4.7 V,*** lithium dendrite or short circuit behavior is detected for the Li|OLiSSE|Li cell after the galvanostatic charge-discharge test for 500 *** fabricated Li|OLiSSE|LiFePO_(4) all-solid-state cell without using any separator and liquid plasticizer directly delivers an initial discharge capacity of 151.4 mAh g^(−1) at the discharge rate of 0.1 C,and shows excellent charge-discharge cycle stability,implying large potential application in the next generation of safe and flexible all-solid-state lithium batteries.

关键词： Solid state electrolytes Organic fast ion-conductor Ordered nano-pathway Electrochemical energy storage ionic conductivity

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Preparation and ionic conductivity of Ultrafine Li_(2+x)RE_xSi_(1-x)O_3 by Sol-Gel Method

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Journal of Rare Earths 2000年第3期18卷 240-243页

作者：陈汝芬宋秀芹贾密英 Department of Chemistry Hebei Normal University Shijiazhuang 050016 China

Li 2+ x RE x Si 1- x O 3(RE=Pr, Nd, Sm, Gd; x =0～0 15) samples were prepared by the sol gel method. DTA TG, XRD, TEM and A C impedance techniques were used to investigate the structure, shape, and ionic conductivity of these samples. The results show that the range of solid solution formation is in 0conductivity of these samples raises with the increasing amount of RE 2O 3 (RE=Pr, Nd, Sm, Gd) added, and the diameter of the powders is about 100 nm. Compared with the conventional solid state reaction, the sol gel method needs low temperature and presents high ionic conductivity.

关键词： rare earths Li 2+ x RE x Si 1- x O 3 (RE=Pr, Nd, Sm, Gd) ionic conductivity sol gel method

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Co-doping strategy enhanced the ionic conductivity and excellent lithium stability of garnet-type Li_(7)La_(3)Zr_(2)O_(12)electrolyte in all solidstate lithium batteries

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Journal of Materiomics 2023年第4期9卷 651-660页

作者： Ziqiang Xu Xin Hu Bowen Fu Kashif Khan Jintian Wu Teng Li Haiping Zhou Zixuan Fang Mengqiang Wu School of Materials and Energy University of Electronic Science and Technology of ChinaChengdu611731SichuanChina Yangtze Delta Region Institute(HuZhou) University of Electronic Science and Technology of ChinaHuzhou313001ZhejiangChina School of Chemical Engineering Sichuan University of Science&EngineeringZigong643000China

Garnet-type Li_(7)La_(3)Zr_(2)O_(12)(LLZO)is one of the most promising solid-state electrolytes(SSEs).However,the application of LLZO is limited by structural instability,low ionic conductivity,and poor lithium *** obtain a garnet-type solid electrolyte with a stable structure and high ionic conductivity,a series of TaeCe co-doping cubic Li_(6.4)La_(3)Zr_(1.4-x)Ta_(0.6)Ce_(x)O_(12)(LLZTCO,x=,0.02,0.04,0.06,0.08,0.10,0.20,0.30)electrolytes were successfully synthesized through conventional solid-phase *** Ta^(5+)doping can introduce more lithium vacancies and effectively maintain the stability of the cubic *** Ce^(4+)with a larger ionic radius is introduced into the lattice to widen the Lit migration bottleneck size,which significantly increased the ionic conductivity to 1.05×10^(-3)S/*** also shows excellent stability to lithium metal by the optimization of Lit transport ***||LLZTCO||Li symmetric cells can cycle stably for more than 6000 h at a current density of 0.1 mA/cm^(2)without any surface *** commercialization potential of LLZTCO samples in all solid-state lithium batteries(ASSLBs)is confirmed by the prepared LiFePO_(4)||LLZTCO||Li cells with a capacity retention rate of 98%after 100 cycles at *** new co-doping method presents a practical solution for the realization of high-performance ASSLBs.

关键词： Solid-state electrolytes Garnet-type Co-doping Bottleneck size ionic conductivity Lithium stability

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A Valence Electron Structure Criterion of ionic conductivity of Sr- and Mg-doped LaGaO_3 Ceramics

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Journal of Materials Science & Technology 2006年第2期22卷 215-219页

作者： Min SHI Ning LIU Yudong XU Can WANG Yupeng YUAN P.Majewski Department of Materials Science and Engineering Hefei University of Technology Hefei 230009 China Max-Planck-Institute for Metals Research Stuttgart 70569 Germany

The valence electron structures of Sr- and Mg-doped LaGaO3 ceramics with different compositions were calculated by Empirical Electron Theory of Solids and Molecules （EET）. A criterion for the ionic conductivity was proposed, i.e. the 1/（nAnB） increases with increasing the ionic conductivity when x or y〈20% （in molar fraction）.

关键词： Empirical electron theory of solids and molecules (EET) Valence electron structure LaGaO3 ceramics ionic conductivity

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