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Journal of Energy Chemistry 2020年第9期29卷 267-276,I0008页

作者： Yan-Qiu Shen Fang-Lei Zeng Xin-Yu Zhou An-bang Wang Wei-kun Wang Ning-Yi Yuan Jian-Ning Ding School of Material Science and Engineering Jiangsu Collaborative Innovation Center of Photovoltaic Science and EngineeringJiangsu Province Cultivation base for State Key Laboratory of Photovoltaic Science and TechnologyChangzhou UniversityChangzhou 213164JiangsuChina Institute of Intelligent Flexible Mechatronics Jiangsu UniversityZhenjiang 212013JiangsuChina Military Power Sources Research and Development Center Research Institute of Chemical DefenseBeijing 100191China

Lithium-sulfur(Li-S)battery can satisfy the need of the future power battery market because of its high energy density,but the hidden dangers caused by lithium anode have seriously hindered their ***,an innovative gel polymer electrolyte(GPE)composed of polyvinylidene fluoride(PVDF)and organo-polysulfide polymer(PSPEG)is proposed,which could be used in semisolid-state Li-S batteries for protection of Li ***,organo-polysulfide polymer could chemically/electrochemically generate both inorganic and organic components simultaneously in-situ once contacting fresh Li metal surface and/or during discharging *** these inorganic/organic components could participate in the formation of the SEI layer and finally constitute a stable and flexible hybrid SEI layer on the surface of Li metal ***,the organic components were permselective to lithium ions against ***,PVDF/PSPEG GPE ensures the ideal chemical and electrochemical properties for Li-S *** work demonstrates an effective solution to solve the problems about Li anodes and contributes to the development of the safe Li metal batteries.

关键词： gel polymer electrolyte Organo-polysulfides Lithium dendrite Solid electrolyte interphase Lithium-sulfur battery

Single-atom electrocatalyst and gel polymer electrolyte boost the energy density and life of aluminum-sulfur batteries

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Journal of Materials Science & Technology 2023年第21期152卷 86-93页

作者： Zheng Huang Wei Wang Mingyin Kou Haiping Lei Yiwa Luo Shuqiang Jiao State Key Laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijing 100083China

Aluminum-sulfur(Al-S)batteries are regarded as a desirable candidate for large-scale energy storage be-cause of their high energy density and abundant natural resources of electrode *** address the critical issues of low discharge voltage and rapid capacity decay in Al-S batteries,here an electrocatalyst-assisted gel-polymer electrolyte(GPE)-based Al-S battery is fabricated using platinum nanoparticles deco-rated platinum/nitrogen co-doped graphene(PtNG)as sulfur host for positive electrode and metal-organic frameworks(MOF)filled GPE(MOF@GPE)as solid ***-based active sites derived from Pt nan-oclusters’surface and atomically dispersed Pt-N_(2) chemical bonds in PtNG can catalyze the decomposition of sulfur and polysulfides in the electrochemical process,greatly accelerating the sulfur redox ***,the MOF fillers in MOF@GPE electrolyte significantly inhibit the shuttle effect of polysul-fides,efficiently improving the utilization of ***,the established Al-S battery delivers a specific capacity of 1009 mAh g^(−1) with a discharge plateau of∼0.95 V,along with a capacity retention of 65% after 300 cycles,revealing ultrahigh energy density and long cycle *** a strategy of combin-ing electrocatalyst and MOF-based gel electrolyte affords a fresh plateau for promoting the rechargeable ability of Al-S batteries,advancing remarkable routes for achieving efficient and stable energy storage devices.

关键词： Aluminum-sulfur batteries gel polymer electrolyte Single atom electrocatalyst Shuttle effect Reaction kinetics

A lithiated gel polymer electrolyte with superior interfacial performance for safe and long-life lithium metal battery

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Journal of Energy Chemistry 2021年第4期30卷 313-322页

作者： Jia-Jia Yuan Chuang-Chao Sun Li-Feng Fang You-Zhi Song Yan Yan Ze-Lin Qiu Yu-Jie Shen Han-Ying Li Bao-Ku Zhu Key Laboratory of Macromolecular Synthesis and Functionalization(Ministry of Education) Department of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027ZhejiangChina Institute of Nuclear and New Energy Technology Tsinghua UniversityBeijing 100084China

Rechargeable lithium metal batteries(LMBs)have gained much attention ***,the short lifespan and safety issues restrict their commercial *** we report a novel gel polymer electrolyte(GPE)based on lithiated poly(vinyl chloride-r-acrylic acid)(PVCAALi)to realize dendritesuppressing and long-term stable lithium metal *** chains ensure the quick gelation process and high electrolyte uptake,and lithiated PAA segments enable the increase of mechanical strength,acceleration of lithium-ion transmission and improvement of interfacial *** GPE showed much higher mechanical strength compared with other free-standing GPEs in previous *** displays a superior ionic conductivity of 1.50 m S cm^(-1) and a high lithium-ion transference number of 0.59 at room ***,the lithiated GPE exhibits excellent interfacial compatibility with lithium metal *** symmetrical cells with PVCAALi GPE yield low hysteresis of 50 m V over1000 h at 1.0 m A cm^(-2).And the possible mechanism of the lithiated GPE with improved lithium-ion transfer and interfacial property was ***,both the Li4Ti5O12/Li and lithium-sulfur(Li-S)cells assembled with PVCAALi GPE show outstanding electrochemical performance,retaining high discharge capacities of 133.8 m Ah g^(-1) and 603.8 m Ah g^(-1) over 200 cycles,*** work proves excellent application potential of the highly effective and low-cost PVCAALi GPE in safe and long-life LMBs.

关键词： Lithiation gel polymer electrolyte Lithium dendrite Safety Lithium metal battery

A UV cross-linked gel polymer electrolyte enabling high-rate and high voltage window for quasi-solid-state supercapacitors

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Journal of Energy Chemistry 2023年第1期76卷 41-50,I0002页

作者： Yuge Bai Chao Yang Boheng Yuan Hongjie Li Weimeng Chen Haosen Yin Bin Zhao Fei Shen Xiaogang Han State Key Laboratory of Electrical Insulation and Power Equipment School of Electrical EngineeringXi'an Jiaotong UniversityXi'an 710049ShaanxiChina Key Laboratory of Smart Grid of Shanxi Province Xian 710049ShaanxiChina

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 ***,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 ***,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.

关键词： gel polymer electrolyte UV cross-linking Energy density High voltage window

PVDF-HFP-SN-based gel polymer electrolyte for high-performance lithium-ion batteries

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Nano Research 2023年第7期16卷 9480-9487页

作者： Ruling Huang Ruochen Xu Jiangtao Zhang Jiayun Wang Tianyi Zhou Mingyi Liu Xiaolong Wang Huaneng Clean Energy Research Institute Beijing 102209China

gel polymer electrolytes(GPEs)have attracted extensive attention in lithium-ion batteries due to their high security and excellent electrochemical ***,their inferior Li-ion transference number,low room-temperature ionic conductivity,and poor long cycle stability raise challenges in practical ***,a flexible poly(vinylidene fluoride-cohexafluoropropylene)-butanedinitrile(PVDF-HFP-SN)-based GPE(PSGPE)is synthesized successfully by a general immersion precipitation *** resultant PSGPEs have numerous connecting pores to ensure sufficient space for liquid ***,the reduced crystallinity of PVDF-HFP and the high polarity of SN can reduce the energy barrier of Li-ions shuttling between *** synergistic effect possesses a high ionic conductivity of 1.35 mS·cm^(-1)at room temperature with a high Li-ion transference number of *** PVDF-HFP-SN-based GPE is applied in a LiFePO_(4)/graphite battery,which can realize stable cycling performance for 350 cycles and good rate performance at room *** results demonstrate that the novel PSGPE possesses advantage in simplified production process,which can improve the practicability of gel polymer lithium-ion batteries.

关键词： poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP)-based butanedinitrile(SN) gel polymer electrolyte synergistic effect

PVdF-HFP-Based gel polymer electrolyte with Semi-Interpenetrating Networks For Dendrite-Free Lithium Metal Battery

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Acta Metallurgica Sinica(English Letters) 2021年第3期34卷 417-424页

作者： Lu Liu Xiaodong Wang Chenhui Yang Peng Han Lei Zhang Li Gao Zirui Wu Bingxin Liu Ruiping Liu Department of Materials Science and Engineering China University of Mining and Technology(Beijing)Beijing 100083.China Department of Mechanical Engineering University of Alaska FairbanksFairbanksAK 99775-5905USA School of Mechanical Engineering Qinghai UniversityXining 810016China

The safety issues and lower energy density of the lithium metal batteries are the two main challenges that hinder their applications in the fields of electric vehicles and portable *** this work,the semi-interpenetrated polyvinylidene fluoride-hexafluoropropylene(PVdF-HFP)-based gel polymer electrolyte was synthesized through UV-curing method by employing the ethoxylated trimethylolpropane triacrylate(ETPTA)*** semi-interpenetrating networks formed by polymerization of ETPTA and the high liquid absorption rate of the PVdF-HFP impart the as-prepared electrolyte with a high room temperature ionic conductivity of 3.17×10-3 s cm^(-1)and a high mechanical strength of 3.46 ***4 was selected as cathode materials,and the active material loading of the cathode is about 4.2 mg *** electrolyte shows superior long-term cycling properties(127 mAh g^(-1)after 200 cycles at 0.5 C),excellent rate performance(113 mAh g^(-1)at1 C,80 mAh g^(-1)at 2 C,and the discharge capacity of 135 mAh g^(-1)can be restored when the rate goes back to 0.1 C)as well as good ability to inhibit the growth of lithium dendrite(about 150 h).The facile synthesis strategy and great electrochemical performance of the electrolyte make it a potential candidate for lithium metal batteries.

关键词： gel polymer electrolyte PVdF-HFP UV-curing Lithium dendrite

Asymmetric fireproof gel polymer electrolyte constructed by boron-contained covalent organic framework for dendrite-free sodium metal battery

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Nano Research 2024年第11期17卷 9679-9687页

作者： Zhanming Liu Rui Wang Jiayi Yu Zhengrui Miao Zijian Xu Jianguo Ren Suli Chen Tianxi Liu Key Laboratory of Synthetic and Biological Colloids Ministry of Education School of Chemical and Material Engineering Jiangnan University Wuxi 214122 China BTR New Material Group Co. Ltd. Shenzhen 518000 China

gel polymer electrolytes (GPEs) with flexibility, easy processability, and low cost have been regarded as promising alternatives for conventional liquid electrolytes in next-generation sodium metal batteries (SMBs). However, GPEs often suffer from combustion risk and inferior interfacial compatibility toward Na metal anode, which severely limit their wide commercial applications. Here, a rational design of asymmetric fireproof GPE (AFGPE) modified with a boron-contained covalent organic framework (BCOF) on one side is developed through in-situ crosslinking polymerization process. Benefiting from the unique structure and composition, the resulting AFGPE exhibits high Na+ transference number, wide electrochemical window, excellent mechanical properties and high safety. Especially, the nanoscale BCOF layer with uniform nanochannels works as ion sieve that homogenizes Na+ flux during Na plating process, while the abundant Lewis-acid B sites can strongly capture counter anions and decrease space charge layer at anode side, thus promoting the uniform Na deposition to effectively suppress dendrite growth. Consequently, the Na/AFGPE/Na symmetric cells demonstrate remarkable cycling stability for over 1200 h at 0.1 mA·cm^(-2), and the solid-state SMBs exhibit outstanding cycling properties and rate capability, delivering a high capacity retention of 96.4% under current density of 1 C for over 1000 cycles.

关键词： gel polymer electrolyte sodium metal battery covalent organic framework flame-retardant interfacial stability

High-performance PVDF-HFP based gel polymer electrolyte with a safe solvent in Li metal polymer battery

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Journal of Energy Chemistry 2020年第10期29卷 80-88页

作者： Jing Jie Yulong Liu Lina Cong Bohao Zhang Wei Lu Xinming Zhang Jun Liu Haiming Xie Liqun Sun National&Local United Engineering Laboratory for Power Battery Department of ChemistryNortheast Normal UniversityChangchun 130024JilinChina Department of Materials Science and Engineering University of CaliforniaDavis 95616CAUnited States

Poly(vinylidenefluoride-co-hexafluoropropylene)(PVDF-HFP)based gel polymer electrolytes are widely studied owing to their electrochemical stability and high dielectric ***,most gel polymer electrolytes show unsatisfied safety and interface compatibility due to excessive absorption of volatile and flammable liquid ***,by using a safe solvent(N-methyl-2-pyrrolidone)with higher boiling(203℃)and flash points(95℃),we initiatively fabricate a flexible PVDF-HFP based gel polymer *** obtained gel polymer electrolyte demonstrates a high ionic conductivity of 7.24×10^−4 S cm−1,an electrochemical window of 5.2 V,and a high lithium transference number of *** a result,the synthesized polymer electrolyte exhibits a capacity retention of 70%after 500 cycles at 0.5 C,and a discharge capacity of 86 mAh g−1 even at a high current rate of 10 C for LiFePO4 based Li metal ***,a stable Li plating/stripping for more than 500 h is achieved under 0.1 mAh at both room temperature and 70℃.Our results indicate that the PVDF-HFP polymer electrolyte is promising for manufacturing safe and high-performance Li metal polymer batteries.

关键词： gel polymer electrolyte N-methyl-2-pyrrolidone Interface stability Li-ion conduction path

A hybrid lithium sulfonated polyoxadiazole derived single-ion conducting gel polymer electrolyte enabled effective suppression of dendritic lithium growth

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Chinese Chemical Letters 2022年第2期33卷 1025-1031页

作者： Dazhe Li Longbo Luo Jiadeng Zhu Haimei Qin Pengqing Liu Zhaomei Sun Yi Lei Mengjin Jiang College of polymer Science&Engineering Sichuan UniversityChengdu 610065China Chemical Sciences Division Oak Ridge National LaboratoryOak RidgeTN 37831United States State Key Laboratory for Physical Chemistry of Solid Surfaces Fujian Provincial Key Lab of Theoretical and Computational Chemistryand College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

Lithium metal is deemed as an ideal anode material in lithium-ion batteries because of its ultrahigh theoretical specific capacity and the lowest redox ***,the rapid capacity attenuation and inferior security resulting from the dendritic lithium growth severely limit its *** a novel hybrid gel polymer electrolyte (GPE) based on electrospun lithium sulfonated polyoxadiazole (LiSPOD) nanofibrous membrane swelled by lithium bis(trifluoromethanesulfonyl)imide (Li TFSI) ether liquid electrolyte is proposed to address the issue of lithium *** Li-SPOD membrane synthesized by a simple one-pot method exhibits excellent mechanical strength and thermal resistance due to its high molecular weight and rigid *** electron-withdrawing oxadiazole ring and oxadiazole ring-Li;complex,and N,O heteroatoms with lone pairs of electrons in Li-SPOD macromolecular chains facilitate the dissociation of-SO_(3)Li group and Li^(+)*** hybrid Li-SPOD GPE exhibits both a high lithium-ion transference number (0.64) and high ionic conductivity (2.03 m S/cm) as well as superior interfacial compacity with lithium *** Li Fe PO_(4)-Li cell using this novel GPE can operate steadily at 2C for 300 cycles,remaining a high discharge capacity of 125 m Ah/g and dendrite-free *** performance improvements for the Li-Li and Cu-Li cells are also presented.

关键词： Polyoxadiazole sulfonate Single-ion conductor gel polymer electrolyte Lithium dendrite Lithium metal battery

Enhanced performance of solid-state Li–O_2 battery using a novel integrated architecture of gel polymer electrolyte and nanoarray cathode

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Rare Metals 2018年第6期37卷 527-535页

作者： Liang Xiao Er-Wei Li Jing-Yu Yi Wen Meng Bo-Hua Deng Jin-Ping Liu School of Chemistry Chemical Engineering and Life Sciences Wuhan University of Technology State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology

The present work proposes a novel strategy to fabricate an integrated architecture of gel polymer electrolyte （GPE）-nanoarray cathode for lithium-O2 batteries （LOBs）. As a proof-of-concept experiment, the photo-initiated in situ polymerization of GPE was carried out via incorporating the precursor solution in advance into a self- standing binder-free oxygen electrode of Co3O4 nanosheets array grown on carbon cloth （Co3O4@CC）, forming an integrated GPE-Co3O4@CC architecture. The performance of the solid-state LOBs using the GPE-Co3O4@CC assembly is greatly enhanced compared to the counterparts with a traditional cell structure, in which GPE was sandwiched by a lithium metal and a cathode. The enhanced performance is ascribed to the combination of the in situ polymerization of GPE and the versatile structure of nanoarray electrode, which results in abundant interfacial contacts between GPE and electrode. This work presents an alternative way to develop high-performance solid-state LOBs by combining the advantages of both gel polymer electrolytes and nanoarray electrodes.

关键词： Solid-state Li-O2 battery gel polymer electrolyte Co3O4 nanosheet Nanoarray electrode electrolyte-cathode interface