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science China(Technological sciences) 2022年第7期65卷 1567-1577页

作者： XIONG DongGen XU ling XU Jian ZHANG XiangXiang li Jia XU YuQing ZHANG Ze YU Ji YANG ZhenYu Key Laboratory of Jiangxi Province for Environment and Energy Catalysis College of ChemistryNanchang UniversityNanchang 330031China Department of Physics Nanchang UniversityNanchang 330031China

A dual-regulation strategy of adopting B/N codoped carbon nanotube-encapsulated nickel nanoparticles(Ni@BNCNT) as a sulfur host and separator coating is proposed for high-performance Li-S batteries. On the cathode side, the 3D conductive network structure of Ni@BNCNT is favorable for high sulfur utilization, and the collaboration between polar metal Ni nanoparticles(NPs) and doped B/N elements facilitates the chemical adsorption of li polysulfides(li Pss). In addition, these metal Ni NPs exhibit a satisfactory catalytic effect on the polysulfide conversion. Moreover, using the Ni@BNCNT interlayer can further capture the soluble li Pss, make them convert quickly, and prevent them from diffusing toward the anode side. The Li-S batteries simultaneously equipped with a s/Ni@BNCNT cathode and Ni@BNCNT interlayer show high reversible capacity and good cycle stability. Additionally, even at a sulfur loading of 3.5 mg cm;and an electrolyte/sulfur ratio of 3 μL mg;, excellent battery performance can be achieved. We believe that this work offers a new strategy based on combining a catalytic host and separator coating to construct high-efficiency Li-S batteries.

关键词： Li-S batteries CNT-encapsulated Ni catalysts dual-regulation strategy catalytic host separator coating

A semi-immobilized sulfur-rich copolymer backbone with conciliatory polymer skeleton and conductive substrates for high-performance Li-S batteries

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能源化学:英文版 2023年第6期81卷 510-518,I0012页

作者： Tianpeng Zhang Zihui song Jinfeng Zhang Wanyuan Jiang Runyue Mao Borui li siyang liu Xigao Jian Fangyuan Hu school of Materials science and Engineering State Key Laboratory of Fine ChemicalsFrontiers Science Center for Smart Materials Oriented Chemical EngineeringTechnology Innovation Center of High Performance Resin Materials(Liaoning Province)Key Laboratory of Energy Materials and Devices(Liaoning Province)Dalian University of TechnologyDalian 116024LiaoningChina school of Chemical Engineering State Key Laboratory of Fine ChemicalsFrontiers Science Center for Smart Materials Oriented Chemical EngineeringTechnology Innovation Center of High Performance Resin Materials(Liaoning Province)Key Laboratory of Energy Materials and Devices(Liaoning Province)Dalian University of TechnologyDalian 116024LiaoningChina

sulfur-rich polymers have gained a great deal of attention as the next-generation active materials in lithium-sulfur(li-s)batteries due to their low cost,environmental compatibility,naturally sulfur uniform dispersion,and distinctive structure covalently bonding with sulfur atoms.However,the poor electrical conductivity and undesirable additional shuttle effect still hinder the commercial application of sulfur-rich polymers.Herein,we report a flexible semi-immobilization strategy to prepare allylterminated hyperbranched poly(ethyleneimine)-functionalized reduced graphene oxide(A-PEI-EGO)as sulfur-rich copolymer backbone.The semi-immobilization strategy can effectively reconcile the demand for polymer skeleton and conductive substrates through forming quaternary ammonium groups and reducing oxygen-containing functional groups,resulting in enhanced skeleton adsorption capacity and substrate electronic conductivity,respectively.Furthermore,the stable covalent bonding connection based on polymer molecules(A-PEI)not only completely prevents the additional shuttle effect of lithiation organic molecules and even sulfur-rich oligomers,but provides more inverse vulcanization active sites.As a result,the as-prepared A-PEI-EGO-s cathodes display an initial discharge capacity of1338 m A h g^(-1)at a rate of 0.1 C and an outstanding cycling stability of 0.046%capacity decay per cycle over 600 cycles.Even under 6.2 mg cm^(-2)s-loaded and sparing electrolyte of 6μL mg^(-1),the A-PEI-EGO-s cathode can also achieve a superior cycling performance of 98%capacity retention after 60 cycles,confirming its application potential.

关键词： Li-S batteries sulfur-rich polymers semi-immobilization strategy Demand reconciliation Outstanding cycling stability

Enhanced catalytic conversion of polysulfides using high-percentage 1T-phase metallic Ws_(2) nanosheets for li–s batteries

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Green Energy & Environment 2022年第6期7卷 1340-1348页

作者： Changyu Yang Ning Gong Tao Chen Yang li Wenchao Peng Fengbao Zhang Xiaobin Fan school of Chemical Engineering and Technology State Key Laboratory of Chemical EngineeringCollaborative Innovation Center of Chemical Science and EngineeringTianjin UniversityTianjin300072China

High-energy-density lithium-sulfur batteries has attracted substantial attention as competitive candidates for large-scale energy storage technologies.still,the adverse“shuttle effect”and sluggish sulfur conversion reaction kinetics immensely obstruct their commercial viability.Herein,a two-dimensional metallic 1T phase Ws_(2)(1T-Ws_(2))nanosheets modified functional separator is developed to improve the electrochemical performance.Meanwhile,the semiconducting bulk-Ws_(2) crystals,and 2H phase Ws_(2)(2H-Ws_(2))nanosheets with more basal-plane svacancy defects are also prepared to probe the contributions of the crystal structure(phase),s-vacancy defects,and edges to the li–s batteries performance experimentally and theoretically.In merits of the synergistic effect of high ion and electron conductivity,enhanced binding ability to lithium polysulfides(liPss),and sufficient electrocatalytic active sites,the 1T-Ws_(2) shows highly efficient electrocatalysis of liPss conversion and further improves li–s battery performance.As expected,thus-fabricated cells with 1T-Ws_(2) nanosheets present superior cycle stability that maintain capacity decline of 0.039%per cycle after 1000 cycles at 1.0 C.The strategy presented here offers a viable approach to reveal the critical factors for liPss catalytic conversion,which is beneficial to developing advanced li–s batteries with enhanced properties.

关键词： Li-S batteries Electrocatalysts Polysulfides Ws_(2)

High-density/efficient surface active sites on modified separators to boost Li-S batteries via atomic Co^(3+)-se termination

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Nano Research 2022年第8期15卷 7199-7208页

作者： shujie liu Xiaofei liu Manfang Chen Dong Wang Xin Ge Wei Zhang Xiyang Wang Chunhui Wang Tingting Qin Haozhe Qin liang Qiao Dan Zhang Xing Ou Weitao Zheng Key Laboratory of Automobile Materials of MOE School of Materials Science and Engineeringand Electron Microscopy Centerand International Center of Future ScienceJilin UniversityChangchun 130013China Key Laboratory of Materials Design and Quantum simulation College of ScienceChangchun UniversityChangchun 130022China National Base for International science&Technology Cooperation School of ChemistryXiangtan UniversityXiangtan 411105China state Key Laboratory of Chem/Bio-sensing and Chemometrics Advanced Catalytic Engineering Research Center of the Ministry of EducationCollege of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China Department of Mechanical and Mechatronics Engineering University of WaterlooWaterlooN2L 3G1Canada school of Metallurgy and Environment Central South UniversityChangsha 410083China

Various and critical electrocatalytic processes are involved during the redox reactions in the Li-S batteries,which extremely depend on the surface structure and chemical state.Recently,single-atom concept unlocks a route to maximize the use of surface-active atoms,however,further increasing the density of active site is still strictly limited by the inherent structure that single-atoms are only highly-dispersed on substrate.Herein,we provide a viewpoint that an elaborate facet design with singlecrystalline structure engineering can harvest high-density surface active sites,which can significantly boost the electrocatalyst performance for excellent Li-S batteries.specifically,the single-crystal Cose_(2)(scCs)exhibits three-types of terminated(011)facet,efficiently obtaining the surface with a high-rich Co^(3+)–se bond termination,in contrast with lots of surface grain boundaries and dangling bonds in polycrystalline Cose_(2).surprisingly,the surface active sites concentration can reach more than 69%.As anticipated,it can provide high-density and high-efficient active sites,enormously suppressing the shuttle effect and improving the reaction kinetics via accelerating the conversion and deposition of polysulfides and li2s.This surface lattice strategy with element terminated mode is a promising approach for designing electrocatalyst effect-based energy system,not merely for Li-S batteries.

关键词： high-density surface active sites Co^(3+)-se covalent bond atomic element terminated Li-S batteries single-crystalline strategy

Direct insight into sulfiphilicity-lithiophilicity design of bifunctional heteroatom-doped graphene mediator toward durable Li-S batteries

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Journal of Energy Chemistry 2022年第3期31卷 474-482,I0013页

作者： Haina Ci Menglei Wang Zhongti sun Chaohui Wei Jingsheng Cai Chen Lu Guang Cui Zhongfan liu Jingyu sun College of Energy Soochow Institute for Energy and Materials InnovationS(SIEMIS)Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu ProvinceSoochow UniversitySuzhou 215006JiangsuChina sUDA-BGI Collaborative Innovation Center Soochow UniversitySuzhou 215006JiangsuChina Beijing Graphene Institute(BGI) Beijing 100095China school of Materials science and Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina Center for Nanochemistry(CNC) Beijing Science and Engineering Center for NanocarbonsCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

The practical applications of lithium-sulfur(li-s)battery have been greatly hindered by the severe polysulfide shuttle at the cathode and rampant lithium dendrite growth at the anode.One of the effective solutions deals with concurrent management of both electrodes.Nevertheless,this direction remains in a nascent stage due to a lack of material selection and mechanism exploration.Herein,we devise a temperature-mediated direct chemical vapor deposition strategy to realize the controllable synthesis of three-dimensional boron/nitrogen dual-doped graphene(BNG)particulated architectures,which is employed as a light-weighted and multi-functional mediator for both electrodes in Li-S batteries.Benefiting from the“sulfiphilic”and“lithiophilic”features,the BNG modified separator not only enables boosted kinetics of polysulfide transformation to mitigate the shuttle effect but also endows uniform lithium deposition to suppress the dendritic growth.Theoretical calculations in combination with electro-kinetic tests and operando Raman analysis further elucidate the favorable sulfur and lithium electrochemistry of BNG at a molecular level.This work offers direct insight into the mediator design via controllable synthesis of graphene materials to tackle the fundamental challenges of Li-S batteries.

关键词： Li-S batteries B/N dual-doped graphene Mediator shuttle effect lithium dendrite

Bidirectional catalysis of Co_(0.4)Ni_(1.6)P for li_(2)s_(1-2) deposition/decomposition reactions in Li-S batteries

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science China Chemistry 2023年第8期66卷 2267-2273页

作者： Luluan Feng shengping Wang Faculty of Materials science and Chemistry China University of GeosciencesWuhan430074China

To improve the electrochemical activity of s electrodes in Li-S batteries,the synergistic electrocatalysis mechanism of Co_(0.4)Ni_(1.6)P with Ni and Co bimetal interactions is clarified.The alternating crystal structure of Co and Ni regulates the adsorption and decomposition energy of Co_(0.4)Ni_(1.6)P to polysulfides and has the bidirectional catalysis for the li_(2)s_(1-2)deposition/decomposition process.Co_(0.4)Ni_(1.6)P can promote the breaking of the s-s bond of li_(2)s_(4) and decrease the decomposition energy barrier of li_(2)s.This regulation accelerates the discharge/charge reaction between s,polysulfides,and li_(2)s and improves the kinetics of the s electrodes.The 1st,100^(th),and 200^(th) discharge capacity densities at 0.1 mA cm^(-2) of the s electrodes with a high sulfur loading were 1,405,987.2,and 828.4 m Ah gs^(-1),respectively.The bidirectional catalytic mechanism is a novel idea for improving the electrochemical performance of Li-S batteries.

关键词： bidirectional catalysis double active sites s electrode separator Li-S batteries

Regulating surface chemistry of separator with liF for advanced Li-S batteries

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Frontiers in Energy 2022年第4期16卷 601-606页

作者： shuai WANG Fanyang HUANG shuhong JIAO Yulin JIE Yawei CHEN shiyang WANG Ruiguo CAO Hefei National Laboratory for Physical science at the Microscale CAS Key Laboratory of Materials for Energy ConversionDepartment of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China

lithium-sulfur(li-s)batteries have attracted intensive attention owing to their ultrahigh theoretical energy density.Nevertheless,the practical application of Li-S batteries is prevented by uncontrollable shuttle effect and retarded reaction kinetics.To address the above issues,lithium fluoride(liF)was employed to regulate the surface chemistry of routine separator.The functional separator demonstrates a great ability to suppress active s loss and protect lithium anode.This work provides a facile strategy for the development of advanced Li-S batteries.

关键词： Li-S batteries liF functional separator

Direct ink writing of metal-based electrocatalysts for li–s batteries with efficient polysulfide conversion

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Interdisciplinary Materials 2023年第4期2卷 589-608页

作者： Ting Meng Zeyu Geng Fei Ma Xiaohan Wang Haifeng Zhang Cao Guan Xi'an Key Laboratory of Flexible Electronics Institute of Flexible ElectronicsNorthwestern Polytechnical UniversityXi'anChina Key laboratory of Flexible Electronics of Zhejiang Province Ningbo Institute of Northwestern Polytechnical UniversityNingboChina

Thanks to the significantly higher energy density compared with universal commercialized li-ion batteries,lithium–sulfur(li–s)batteries are being investigated for use in prospective energy storage devices.However,the inadequate electrochemical kinetics of reactants and intermediates hinder commercial utilization.This limitation results in substantial capacity degradation and short battery lifespans,thereby impeding the battery's power export.Meanwhile,the capacity attenuation induced by the undesirable shuttle effect further hinders their industrialization.Considerable effort has been invested in developing electrocatalysts to fix lithium polysulfides and boost their conversion effectively.In the conventional process,the planar electrodes are prepared by slurry-casting,which limits the electron and ion transfer paths,especially when the thickness of the electrodes is relatively large.Compared with traditional manufacturing methods,direct ink writing(DIW)technology offers unique advantages in both geometry shaping and rapid prototyping,and even complex three-dimensional structures with high sulfur loading.Hence,this review presents a detailed description of the current developments in terms of li–s batteries in DIW of metal-based electrocatalysts.A thorough exploration of the behavior chemistry of electrocatalysis is provided,and the adhibition of metal-based catalysts used for li–s batteries is summarized from the aspect of material usage and performance enhancement.Then,the working principle of DIW technology and the requirements of used inks are presented,with a detailed focus on the latest advancements in DIW of metal-based catalysts in li–s battery systems.Their challenges and prospects are discussed to guide their future development.

关键词： direct ink writing efficient polysulfides conversion Li-S batteries metal-based electrocatalysts

sandwiching sulfur into the Dents Between N,O Co-Doped Graphene Layered Blocks with strong Physicochemical Confinements for stable and High-Rate Li-S batteries

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Nano-Micro Letters 2020年第11期12卷 13-24页

作者： Mengjiao shi su Zhang Yuting Jiang Zimu Jiang Longhai Zhang Jin Chang Tong Wei Zhuangjun Fan Key Laboratory of superlight Materials and surface Technology Ministry of EducationCollege of Material Science and Chemical EngineeringHarbin Engineering UniversityHarbin 150001People’s Republic of China Key Laboratory of Energy Materials Chemistry Ministry of EducationKey Laboratory of Advanced Functional MaterialsAutonomous RegionInstitute of Applied ChemistryXinjiang UniversityUrumqi 830046People’s Republic of China state Key Laboratory of Heavy Oil Processing School of Materials Science and EngineeringChina University of PetroleumQingdao 266580People’s Republic of China

The development of lithium-sulfur batteries(LsBs)is restricted by their poor cycle stability and rate performance due to the low conductivity of sulfur and severe shuttle effect.Herein,an N,O co-doped graphene layered block(NOGB)with many dents on the graphene sheets is designed as effective sulfur host for high-performance LsB s.The sulfur platelets are physically confined into the dents and closely contacted with the graphene scaffold,ensuring structural stability and high conductivity.The highly doped N and O atoms can prevent the shuttle effect of sulfur species by strong chemical adsorption.Moreover,the micropores on the graphene sheets enable fast li^+transport through the blocks.As a result,the obtained NOGB/s composite with 76 wt%sulfur content shows a high capacity of 1413 mAh g^-1 at 0.1 C,good rate performance of 433 mAh g^-1 at 10 C,and remarkable stability with 526 mAh g^-1 at after 1000 cycles at 1 C(average decay rate:0.038%per cycle).Our design provides a comprehensive route for simultaneously improving the conductivity,ion transport kinetics,and preventing the shuttle effect in LsBs.

关键词： Graphene Physicochemical confinement Cycle stability shuttle effect Li-S batteries

CoB and BN composites enabling integrated adsorption/catalysis to polysulfides for inhibiting shuttle-effect in Li-S batteries

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Journal of Energy Chemistry 2021年第8期30卷 220-228,I0005页

作者： Tianli Wu Ting Yang Jizong Zhang Xuewen Zheng Kunlin liu Chengyang Wang Mingming Chen Key Laboratory for Green Chemical Technology of MOE School of Chemical Engineering and TechnologyTianjin University300072 TianjinChina Collaborative Innovation Center of Chemical science and Engineering(Tianjin) 300072 TianjinChina

lithium-sulfur(li-s)batteries are hampered by the infamous shuttle effect and slow redox kinetics,resulting in rapid capacity decay.Herein,a bifunctional catalysis CoB/BN@rGO with integrated structure and synergy effect between adsorption and catalysis is proposed to solve the above problems.The integrated CoB and BN are simultaneously and uniformly introduced on the rGO substrate through a one-step calcination strategy,applied to modify the cathode side of PP separator.The transition metal borides can catalyze the conversion of lithium polysulfides(li_(2)sn,n≥4),whereas the bond of B-s is too weak to absorb LPs.Thus BN introduced can effectively restrict the diffusion of polysulfides via strong chemisorption with lisnli+…N,while the rGO substrate ensures smooth electron transfer for redox reaction.Therefore,through the integrated adsorption/catalysis,the shuttle effect is suppressed,the kinetics of redox reaction is enhanced,and the capacity decay is reduced.Using CoB/BN@rGO modified PP separator,the Li-S batteries with high initial capacity(1450 mAh g^(-1)at 0.35 mA cm^(-2))and long-cycle stability(700 cycles at 1.74 mA cm^(-2)with a decay rate of 0.032%per cycle)are achieved.This work provides a novel insight for the preparation of bifunctional catalysis with integrated structure for long-life Li-S batteries.

关键词： Integrated structure synergy effect Bifunctional catalysis separator Li-S batteries