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In-situ polymerized PEO-based solid electrolytes contribute better Li metal batteries:Challenges,strategies,and perspectives

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Journal of Energy Chemistry 2024年第5期92卷 548-571页

作者： Zhihui Jia Yong Liu Haoming Li Yi Xiong Yingjie Miao Zhongxiu Liu Fengzhang Ren School of Materials Science and Engineering Henan Key Laboratory of Non-Ferrous Materials Science&Processing TechnologyHenan University of Science and TechnologyLuoyang 471023HenanChina Provincial and Ministerial Co-construction of Collaborative Innovation Center for Non-ferrous Metal new Materials and Advanced Processing Technology Henan University of Science and TechnologyLuoyang 471023HenanChina

Polyethylene oxide(PEO)-based solid polymer electrolytes(SPEs)with good electrochemical stability and excellent Li salt solubility are considered as one of the most promising SPEs for solid-state lithium metal batteries(SSLMBs).However,PEO-based SPEs suffer from low ionic conductivity at room temperature and high interfacial resistance with the electrodes due to poor interfacial contact,seriously hindering their practical applications.As an emerging technology,in-situ polymerization process has been widely used in PEO-based SPEs because it can effectively increase Li-ion transport at the interface and improve the interfacial contact between the electrolyte and electrodes.Herein,we review recent advances in design and fabrication of in-situ polymerized PEO-based SPEs to realize enhanced performance in LMBs.The merits and current challenges of various SPEs,as well as their stabilizing strategies are presented.Furthermore,various in-situ polymerization methods(such as free radical polymerization,cationic polymerization,anionic polymerization)for the preparation of PEO-based SPEs are summarized.In addition,the application of in-situ polymerization technology in PEO-based SPEs for adjustment of the functional units and addition of different functional filler materials was systematically discussed to explore the design concepts,methods and working mechanisms.Finally,the challenges and future prospects of in-situ polymerized PEO-based SPEs for SSLMBs are also proposed.

关键词： in-situ polymerization Polyethylene oxide Solid polymer electrolytes Lithium metal anodes

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In-situ construction of PDOL electrolyte with dual-reinforced stable interface for high-voltage lithium metal batteries

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Science China Chemistry 2024年第5期67卷 1664-1671页

作者： Yingkang Wu Yuzhou Bai Wujie Dong Xue Wang Wenqin Ma Fuqiang Huang State Key Lab of Metal Matrix Composites School of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China School of Physical Science and Technology Shanghai Tech UniversityShanghai 201210China Shanghai Institute of Ceramics Chinese Academy of SciencesShanghai 200050China

In-situ polymerized electrolytes significantly enhance the interfacial compatibility of lithium metal batteries(LMBs). Typically,in-situ polymerized 1,3-dioxolane(PDOL) exhibits low interfacial resistance, yet still suffers from low ionic conductivity and a narrow electrochemical stability window(ESW). Here, an ultra-stable PDOL-based polymer electrolyte is developed by incorporating plasticizers of tetramethylene sulfone(TMS) and fluorinated ethylene carbonate(FEC) into the 3D cross-linked network, achieving a significant enhancement in the transport capacity and efficiency of Li-ion. The ionic conductivity reaches3.63×10^(-4)S cm^(-1)even at room temperature, and the transference number(tLi^(+)) is even higher at 0.85. Furthermore, the ESW of this electrolyte can be increased to 4.5 V with the addition of TMS, which forms a thin and robust antioxidant cathode-electrolyte interface(CEI) on the surface of high-voltage LiCoO_(2). FEC generates an inorganic-rich solid-electrolyte interface(SEI) on the Li anode, which effectively inhibits the growth of lithium dendrites. Benefiting from the aforementioned advantages, the highvoltage lithium metal battery demonstrates outstanding long-cycle stability, with 93.2% capacity retention after 200 cycles. This work offers a straightforward and accessible method for the practical implementation of high energy density in-situ polymerized solid-state LMBs.

关键词： solid polymer electrolyte in-situ polymerization PDOL high-voltage LMBs

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In-situ interfacial passivation and self-adaptability synergistically stabilizing all-solid-state lithium metal batteries

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Journal of Energy Chemistry 2024年第1期88卷 282-292,I0007页

作者： Huanhui Chen Xing Cao Moujie Huang Xiangzhong Ren Yubin Zhao Liang Yu Ya Liu Liubiao Zhong Yejun Qiu Shenzhen Engineering Lab of Flexible Transparent Conductive Films School of Materials Science and EngineeringHarbin Institute of TechnologyShenzhen 518055GuangdongChina Guangdong Provincial Key Laboratory of Semiconductor Optoelectronic Materials and Intelligent Photonic Systems School of Materials Science and EngineeringHarbin Institute of TechnologyShenzhen 518055GuangdongChina College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060GuangdongChina School of Resource and Environmental Sciences Wuhan UniversityWuhan 430072HubeiChina

The function of solid electrolytes and the composition of solid electrolyte interphase(SEI)are highly significant for inhibiting the growth of Li dendrites.Herein,we report an in-situ interfacial passivation combined with self-adaptability strategy to reinforce Li_(0.33)La_(0.557)TiO_(3)(LLTO)-based solid-state batteries.Specifically,a functional SEI enriched with LiF/Li_(3)PO_(4) is formed by in-situ electrochemical conversion,which is greatly beneficial to improving interface compatibility and enhancing ion transport.While the polarized dielectric BaTiO_(3)-polyamic acid(BTO-PAA,BP)film greatly improves the Li-ion transport kinetics and homogenizes the Li deposition.As expected,the resulting electrolyte offers considerable ionic conductivity at room temperature(4.3 x 10~(-4)S cm^(-1))and appreciable electrochemical decomposition voltage(5.23 V)after electrochemical passivation.For Li-LiFePO_(4) batteries,it shows a high specific capacity of 153 mA h g^(-1)at 0.2C after 100 cycles and a long-term durability of 115 mA h g^(-1)at 1.0 C after 800 cycles.Additionally,a stable Li plating/stripping can be achieved for more than 900 h at 0.5 mA cm^(-2).The stabilization mechanisms are elucidated by ex-situ XRD,ex-situ XPS,and ex-situ FTIR techniques,and the corresponding results reveal that the interfacial passivation combined with polarization effect is an effective strategy for improving the electrochemical performance.The present study provides a deeper insight into the dynamic adjustment of electrode-electrolyte interfacial for solid-state lithium batteries.

关键词： Solid-state lithium batteries Composite solid electrolyte in-situ polymerization Interfacial passivation layer Self-adaptability

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In situ polymerization preparation and mechanical properties of nanocomposites based on PA10T/10I-block-PEG copolymer and graphene oxide

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Nano Materials Science 2022年第3期4卷 276-284页

作者： Xiao-bo Fu Xin Tong Jia-cao Yang Gang Zhang Mei-lin Zhang Xiao-jun Wang Jie Yang College of Polymer Science and Engineering Sichuan UniversityChengdu610065China Analytical and Testing Center Sichuan UniversityChengdu610064China Jiangsu JITRI Advanced Polymer Materials Research Institute Co. LtdChina State Key Laboratory of Polymer Materials Engineering Sichuan UniversityChengdu610065China

Poly(decamethylene terephthalamide/decamethylene isophthalamide)-block-polyvinyl alcoho)(PA10 T/10 IPEG) copolymer/graphene oxide(GO) composites were prepared via in-situ melt polymerization and two different nano-filler addition approaches were compared. The relationship between the micro-structure and performance of the elastomer composites prepared by one-step and two-step methods was explored. The results show that the two-step method significantly promoted the dispersion of the GO in a polymer matrix, and facilitated the grafting of more hard molecular chains. Thus, the elastic modulus and tensile strength of the nanocomposite have been significantly improved by the presence of GO. This was because of the strong interaction between the functional groups on the surface of the GO and the hard molecular chains. This would be also be favorable to load transfer across the interface. Additionally, the elongation at the break of composites increased by 10% with the addition of a small amount of GO(0.2% wt). This is because hard domains tend to be enriched on the surface of GO in composites and act as a lubricating layer at the interface between the GO and matrix, leading to increased deformation ability. This work provides an effective strategy to prepare elastomer composites with high strength and toughness.

关键词： Graphene oxide Thermoplastic elastomer in-situ polymerization Composite

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Introducing electrolytic electrochemical polymerization for constructing protective layers on Ni-rich cathodes of Li-ion batteries

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Rare Metals 2024年第6期43卷 2536-2545页

作者： Lin-Tao Dou Bei Li Hao-Long Nie Dong-Dong Xiao Chao-Qun Shang Xiao-Min Wang Zhan-Hui Zhang Katerina E.Aifantis Pu Hu School of Materials Science and Engineering Wuhan Institute of Technology Huairou Division Institute of PhysicsChinese Academy of Sciences Department of Mechanical and Aerospace Engineering University of Florida

LiNi0.8Co0.1Mn0.1O2（NCM811） is the most promising cathode for high-energy Li-ion batteries,despite its poor cycling stability that originates from the reactions that occur with the electrolyte.Herein,to solve this interfacial issue,a facile electrolytic electrochemical polymerization process was introduced in this paper,and a uniform conductive electrolyte interface（polyaniline） was successfully constructed on the surface of the NCM811 porous electrode（PANI-NCM）,which facilitated the charge transfer during charge/discharge.The side reactions at the interface between the cathode and the electrolyte are suppressed,and thereby,the cycling performance and rate capability are considerably improved.PANI-NCM delivers an initial capacity of 157.2 mAh·g-1as well as excellent cyclability（capacity retention of 88% after 500 cycles at 2C）,whereas the capacity of the bare NCM811 has dropped to 31.3 mAh·g-1.In addition,polypyrrole and polythiophene also can be formed through electrolytic electrochemical polymerization process,which provides a practicable tactic to modify the interfacial stability of cathodes for high-energy Li-ion batteries.

关键词： Lithium-ion battery Ni-rich cathode in-situ polymerization Conductive polymer Electrochemical performance

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Surface Morphology and Thermo-Electrical Energy Analysis of Polyaniline (PANI) Incorporated Cotton Fabric

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Energy Engineering 2024年第1期121卷 1-12页

作者： Md.Shohan Parvez Md.Mustafizur Rahman Mahendran Samykano Mohammad Yeakub Ali Automotive Engineering Research Group Faculty of Mechanical and Automotive Engineering TechnologyUniversiti Malaysia Pahang Al-Sultan AbdullahPekanMalaysia Department of Textile Engineering Khulna University of Engineering&Technology(KUET)KhulnaBangladesh Centre for Research in Advanced Fluid and Processes(CARIFF) Universiti Malaysia Pahang Al-Sultan AbdullahLebuhraya Tun RazakGambangMalaysia Mechanical Engineering Programme Area Faculty of EngineeringUniversiti Teknologi BruneiBruneiDarussalam

With the exponential development in wearable electronics,a significant paradigm shift is observed from rigid electronics to flexible wearable devices.Polyaniline(PANI)is considered as a dominant material in this sector,as it is endowed with the optical properties of both metal and semiconductors.However,its widespread application got delineated because of its irregular rigid form,level of conductivity,and precise choice of solvents.Incorporating PANI in textile materials can generate promising functionality for wearable applications.This research work employed a straightforward in-situ chemical oxidative polymerization to synthesize PANI on Cotton fabric surfaces with varying dopant(HCl)concentrations.Pre-treatment using NaOH is implemented to improve the conductivity of the fabric surface by increasing the monomer absorption.This research explores the morphological and structural analysis employing SEM,FTIR and EDX.The surface resistivity was measured using a digital multimeter,and thermal stability is measured using TGA.Upon successful polymerization,a homogenous coating layer is observed.It is revealed that the simple pre-treatment technique significantly reduces the surface resistivity of Cotton fabric to 1.27 kΩ/cm with increasing acid concentration and thermal stability.The electro-thermal energy can also reach up to 38.2°C within 50 s with a deployed voltage of 15 V.The modified fabric is anticipated to be used in thermal regulation,supercapacitor,sensor,UV shielding,antimicrobial and other prospective functional applications.

关键词： Polyaniline cotton in-situ polymerization SEM TGA heating fabric

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Surface control of layered double hydroxides by in-situ initiating&terminating polymerization

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Nano Research 2022年第2期15卷 1538-1546页

作者： Dan Tong Yuquan Zhu Kaitao Li Kuilin Du Wendi Liu Yanjun Lin State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China School of Chemical Engineering Qinghai UniversityXining 810016China

Appropriate surface modification or functionalization is prerequisite for the application of inorganic nanoparticles.And surface control between organic and inorganic interface plays an important role in constructing organic-inorganic composites.in-situ polymerization has been extensively studied to improve the compatibility and dispersibility of inorganic nanoparticles,but the polymerized nanoparticles tend to concatenate and form large composites,restricting further applications.Herein,uniform and dense polyacrylic acid(PAA)membranes have been grafted on layered double hydroxide(LDH)nanosheets via an in-situ initiating and terminating radical graft polymerization method.With initiating and terminating on the same particle,the size,morphology and density of grafted PAA onto the surface of LDHs can be controlled by adjusting the ratio of initiated sites to terminated sites,the amount of redox initiator or monomer.As a result,with only 17.33%organic grafting ratio,PAA@LDHs with largely improved compatibility can be monodispersed in polyethylene(PE)and polyvinyl chloride(PVC)matrices,which is determined by a fluorescence microscope technique.

关键词： surface control in-situ polymerization organic-inorganic interface layered double hydroxides

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SYNTHESIS AND CHARACTERIZATION OF POLYPROPYLENE/MONTMORILLONITE NANOCOMPOSITES VIA AN in-situ polymerization APPROACH

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Chinese Journal of Polymer Science 2003年第4期21卷 413-418页

作者：张学全 Changchun Institute of Applied Chemistry Chinese Academy of Sciences Changchun 130022 China

Polypropylene/montmorillonite (PP/MMT)nanocomposites were prepared by in-situ polymerization using aMMT/MgCl_2/TiCl_4-EB Ziegler-Natta catalyst activated by triethylaluminum(TEA). The enlarged layer spacing of MMT wasconfirmed by X-ray wide angle diffraction (WAXD), demonstrating that MMT were intercalated by the catalyst components.X-ray photoelectron spectrometry (XPS) analysis proved that TiCl_4 was mainly supported on MgCl_2 instead of on the surfaceof MMT The exfoliated structure of MMT layers in the PP matrix of PP/MMT composites was demonstrated by WAXDpatterns and transmission electron microscopy (TEM) observation. The higher glass transition temperature and higher storage modulus of the PP/MMT composites in comparison with pure PP were revealed by dynamic mechanical analysis (DMA).

关键词： Polypropylene Nanocomposite in-situ polymerization

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Screening the Insecticidal Efficacy of Nano ZnO Synthesized via in-situ polymerization of Crosslinked Polyacrylic Acid as a Template

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Journal of Materials Science & Technology 2012年第11期28卷 961-968页

作者： M. Mekewi Ahmed Shebl A.I. Imam M.S. Amin T. Albert Chemistry Department Faculty of Science Ain Shams University Plants Protection Department Desert Research Center

Nano zinc oxide （ZnO） is a very useful and important material in many industrial and biological applications. In the present work, ZnO was synthesized by post thermal degradation of the precursor ＂zinc acetate di-hydrate＂ templated in crosslinked polyacrylic acid （PAA）. The crosslinked PAA template was prepared through an in-situ polymerization process adopted in presence of ammonium per sulphate, as an initiator, and N, Nt- methylene bis-acrylamide as the crosslinker. Variation of preparation parameters and their impact on the oxide stoichiometry, crystal structure, crystallite size and surface texture of the oxide were investigated. Energy dispersive X-ray technique （EDX）, X-ray diffraction （XRD） and scanning electron microscopy （SEM） were convincingly used to reveal the oxide structural features and characteristics. The performed bioassay tests indicated the efficacy of this method of preparation to produce nano ZnO with novel insecticidal activity against the greater wax moth, Galleria rnellonella.

关键词： Nano ZnO in-situ polymerization Polymer template Insecticide Bioassay Galleria mellonella

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Preparation of pH-Responsive Doxorubicin Nanocapsules by Combining High-gravity Antisolvent Precipitation with in-situ polymerization for Intracellular Anticancer Drug Delivery

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Chemical Research in Chinese Universities 2020年第5期36卷 927-933页

作者： LIU Jie CHEN Bo ZHANG Jianjun College of Chemical Engineering Beijing University of Chemical TechnologyBeijing 100029P.R.China State Key Laboratory of NBC Protection far Civilian Beijing 102205P.R.China

Owing to the low pH value in tumor and cancer cells,drug delivery systems based on pH-responsive polymer nanocarriers have been extensively explored for anticancer chemotherapy.Herein,we developed a pH-responsive doxonibicin(EXDX)nanocapsule(named as DNanoCapsule)prepared by combining in-situ polymerization teclinique with high-gravity antisolvent precipitation technique throngh an amphiphilic polymerized surface ligand.DNanoCapsules show an obvious spherical core-shell structure with a single DOX nanoparticle encapsulated in the polymer layer.Dissolution rate studies prove that the DNanoCapsules have robust dnig-release profiles under acidic environments due to the division of the pH-sensitive cross-linker,which triggers thecollapse of the polymer layer.The in vitro investigations demonstrated that the DNanoCapsules exhibited higli cellular uptake efficiency and cytotoxicity for both HeLa and MCF-7 cancer cells.Tlierefore,this work may provide a promising strategy to design and develop various stimuli-responsive drug nanocapsules tor the treatment of cancer or other diseases.

关键词： pH-Responsive Nanocapsule in-situ polymerization High-gravity anti solvent precipitation Anticancer cheniotherapy

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