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sulfur-containing polymer cathode materials: From energy storage mechanism to energy density

InfoMat 2022年第8期4卷 1-24页

作者： Rong Zou Wenwu Liu Fen Ran State Key Laboratory of Advanced Processing and Recycling of Non-ferrous Metals School of Material Science and EngineeringLanzhou University of TechnologyLanzhouP.R.China

Besides lithium-ion batteries, it is imperative to develop new battery energystorage system with high energy density. In conjunction with the developmentof Li-S batteries, emerging sulfur-containing polymers with tunable sulfur-chain length and organic groups gradually attract much attention as cathodematerials. This can avoid the problems that are impeding the development ofthe typical Li-S batteries, such as volume expansion, active material dissolu-tion, shuttle effect, and so on. This review aims to generalize the type ofsulfur-containing polymers and the working principles in Li-S batteries. Thesulfur-containing polymers (R-Sn-R) with different sulfur-chain length (n > 6,n ≤ 2, and 3 ≤ n ≤ 6) are summarized. It also discusses several organic groupssuch as phenyl rings, N-heterocycles, and unique structure with cross-linkednetworks and multi-micropores skeleton. This review also explores other strat-egies of sulfur-containing polymers in the rest of Li-S batteries, providing asummary of the advantages of sulfur-containing polymers, recent develop-ment, in-depth discussion of the mechanism in Li-S batteries, and organicgroup-structure-performance relationship. This review would have guidelinesfor future development of sulfur-containing polymers in Li-S batteries.

关键词： cathode materials energy density energy storage mechanism Li-S batteries sulfur-containing polymer

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Selenium-doped cathode materials with polyaniline skeleton for lithium-organosulfur batteries

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Journal of Energy Chemistry 2023年第4期79卷 148-157页

作者： Rong Zou Wenwu Liu Fen Ran State Key Laboratory of Advanced Processing and Recycling of Non-ferrous Metals School of Materials Science and EngineeringLanzhou University of TechnologyLanzhou 730050GansuChina

sulfur-containing polymer(SCP)is considered as an outstanding cathode material for lithium-sulfur ***,undesirable soluble polysulfides may shuttle in electrolyte,concluding long-chain Li_(2)S_(n)(n>4)and short-chain Li2Sn(n≤4),as well as the sluggish conversion kinetics are yet to be solved to enhance the performance of lithium-sulfur *** Se-doped sulfurized polyaniline with adjusted sulfur-chain-S_(x)-(x≤6)contribute to ensure the absence of long-chain polysulfides,and the skeleton with quinoid imine can endow strongly adsorption towards short-chain polysulfides by the reversible transition between deprotonated/protonated imine(-NH^(+)=and-N=),which offer double insurance against suppressing“shuttle effect”.Furthermore,Se atoms are doped into sulfurized polysulfides to accelerate the redox conversion and take a frontier orbital theory-oriented view into catalytic ***-doped sulfurized polyaniline as active materials for lithium-organosulfur batteries delivers good electrochemical performance,including high rate,reversible specific capacity(680 mA h g^(-1)at 0.1 A g^(-1)),and lower capacity decay rate only of 0.15%with near 100%coulomb efficiency during long-term *** work provides a valuable guiding ideology and promising solution for the chemistry-oriented structure design and practical application for lithium-organosulfur batteries.

关键词： Lithium-organosulfur batteries Selenium-doped Cathode materials sulfur-containing polymer Frontier orbital theory

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Dynamic sulfur-Rich polymers from Elemental sulfur and Epoxides

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Chinese Journal of polymer Science 2024年第10期42卷 1479-1487,I0010页

作者： Ke-Xiang Chen Chen-Hui Cui Zhen Li Ting Xu Hao-Qing Teng Zhi-Yuan He Yin-Zhou Guo Xiao-Qing Ming Zhi-Shen Ge Yan-Feng Zhang Tie-Jun Wang School of Chemistry Engineering Research Center of Energy Storage Materials and DevicesMinistry of EducationXi’an Jiaotong UniversityXi’an710049China State Key Lab for Strength and Vibration of Mechanical Structures Department of Engineering MechanicsXi’an Jiaotong UniversityXi’an710049China

sulfur-containing dynamic polymers had attracted significant attention due to their unique chemical structures with high *** sulfur, an inexpensive industrial waste product, to synthesize dynamic polysulfide polymers through reverse vulcanization has been a notable approach. However, this method required high temperatures and resulted in the release of unpleasant oders. In this study, we presented a robust method for the preparation of sulfur-rich polymers with dynamic polysulfide bonds from elemental sulfur and inexpensive epoxide monomers via a one-pot strategy at the mild room temperature. Different types of polysulfide molecules and polymers were synthesized by reacting various epoxide compounds with sulfur, along with the investigation of their structures and dynamic behaviors. It was noteworthy that the obatined polymers prepared from m-(2,3-epoxypropoxy)-N,N-bis(2,3-epoxypropyl)aniline and elemental sulfur exhibit multiple dynamic behaviors, including polysulfide metathesis and polysulfide-thiol exchange, enabling their rapid stress relaxation, self-healing, reprocessing and degradable properties of the cross-linked polymer. More importantly, the hydroxyl groups at the side chains from epoxide ring opening exhibited potential transesterification. This work provided a facile strategy for designing dynamic sulfur-rich polymers via a mild synthesis route.

关键词： Elemental sulfur sulfur-containing polymer Dynamic covalent bond Dynamic polymer

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Anionic Copolymerization of Carbonyl Sulfide with Epoxides via Alkali Metal Alkoxides

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Chinese Journal of Chemistry 2018年第7期36卷 625-629页

作者： Cheng-Jian Zhang Jia-Liang Yang Lan-Fang Hu Xing-Hong Zhang MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou Zhejiang 310027 China

Carbonyl sulfide （COS）, an analogue of carbon dioxide （CO2）, can be converted to CO2 via the carbonic anhydride enzymes widely existing in nature. COS is an ideal monomer for making poly（monothiocarbonate）s, which are difficult to synthesize by traditional methods. Herein, for the first time, we describe an anionic copolymerization of COS with epoxides using alkali metal alkoxides as the catalysts （initiators）, affording poly（monothiocarbonate）s with 100% alternating degree, 〉99% tail-to-head （T-H） content, high number-average molecular weights （Mns, up to 90.3 kg/mol） with narrow molecular weight distributions （D=Mw/Mn, 1.05-1.31 for COS/propylene oxide copolymers） under solvent-free and mild conditions. Oxygen-sulfur exchange reaction （O/S ER）, which can result in the production of contaminated dithiocarbonate and carbonate units in the main chain, was nearly completely depressed at 0 ℃. In addition, in contrast to previously reported salen chromium （iron） complexes that required multiple synthetic steps, this work provides simple, low-cost, and effective catalysts for making colorless sulfur-containing polymers.

关键词： carbonyl sulfide copolyrnerization alkali metal alkoxides sulfur-containing polymer

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DFT-supported Mechanistic Understanding of the Ring-opening polymerization of Cyclic Trithiocarbonates Mediated by Organic Base

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Chemical Research in Chinese Universities 2023年第5期39卷 772-776页

作者： WANG Xinjie REN Baihao ZHAO Jinzhuo YUE Tianjun KANG Xiaohui REN Weimin State Key Laboratory of Fine Chemicals Frontiers Science Center for Smart MaterialsDalian University of TechnologyDalian 116024P.R.China College of Pharmacy Dalian Medical UniversityDalian 116044P.R.China

sulfur-rich polymers are endowed with several enhanced features,such as high refractive index and excellent thermal and mechanical properties,owing to the incorporation of sulfur atoms into the polymer main *** an important category of sulfur-rich polymers,polytrithiocarbonates can be efficiently synthesized through ring-opening polymerization(ROP)of cyclic trithiocarbonates(CTCs)mediated by 1,5,7-triazabicyclo[4.4.0]dec-5-ene(TBD)and benzyl mercaptan(BnSH).However,the mechanistic investigations of this reaction are *** this study,we attempted to understand this reaction by simulating chain initiation,propagation,and termination in the ROP of CTCs using density functional theory(DFT)*** demonstrated,the acceleration of the ROP ofδ-CTC by BnSH can be attributed to the smaller size of BnS-compared to TBD when nucleophilic attacking,and[TBDH]+enhancing the interaction with the monomer and stabilizing the generated active species in the initiating *** addition,the ability of BnSH to tune the topological structures of the final polymers is ascribed to the suppressed transesterification between the thiolate species and the first trithiocarbonate unit initiated by BnS-.Furthermore,the limitations that hinder the ROP of five-and six-membered CTCs under general conditions are the unfavored thermodynamic factors,wherein the ROP of six-membered CTC is possible below-75℃.

关键词： Cyclic trithiocarbonate Density functional theory calculation Ring-opening polymerization sulfur-containing polymer

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