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sulfur polymerization strategy based on the intrinsic properties of polymers for advanced binder-free and high-sulfur-content li–s batteries

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susMat 2023年第1期3卷 111-127页

作者： Zihui song Tianpeng Zhang siyang liu Wenlong shao Wanyuan Jiang Runyue Mao 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 TechnologyDalianChina state Key Laboratory of Fine Chemicals Frontiers Science Center for Smart Materials Oriented Chemical EngineeringSchool of Chemical EngineeringTechnology Innovation Center of High Performance Resin Materials(Liaoning Province)Key Laboratory of Energy Materials and Devices(Liaoning Province)Dalian University of TechnologyDalianChina

lithium-sulfur(li-s)batteries are the promising next-generation secondary energy storage systems,because of their advantages of high energy density and environmental friendliness.Among numerous cathode materials,organosulfur polymer materials have received extensive attentions because of their controllable structure and uniform sulfur distribution.However,the sulfur content of most organosulfur polymer cathodes is limited(s contents of conductive agents and binders,which adversely affects the energy density of li-s batteries.Herein,a hyperbranched sulfur-rich polymer based on modified polyethyleneimine(Ath-PEI)named carbon nanotubeentangled poly(allyl-terminated hyperbranched ethyleneimine-random-sulfur)(CNT/Ath-PEI@s)was prepared by sulfur polymerization and used as a li-s battery cathode.The high intrinsic viscosity of Ath-PEI provided considerable adhesion and avoided the addition of PVDF binder,thereby increasing the sulfur content of cathodes to 75%.Moreover,considering the uniform distribution of elemental sulfur by the polymer,the utilization of sulfur was successfully improved,thus improving the rate capability and discharge capacity of the battery.The binder-free,sulfur-rich polymer cathode exhibited ultra-high initial discharge capacity(1520.7 mAh g^(−1) at 0.1 C),and high rate capability(804 mAh g^(−1) at 2.0 C).And cell-level calculations show that the electrode exhibits an initial capacity of 942.3 mAh g^(−1) electrode,which is much higher than those of conventional sulfur-polymer electrodes reported in the literature.

关键词： high sulfur content intrinsic viscosity li-s batteries organosulfur polymers sulfur uniform distribution

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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

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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

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MoP QDs@graphene as highly efficient electrocatalyst for polysulfide conversion in li-s batteries

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Journal of Materials science & Technology 2021年第31期90卷 37-44页

作者： Bo Yu Fei Ma Dongjiang Chen Katam srinivas Xiaojuan Zhang Xinqiang Wang Bin Wang Wanli Zhang Zegao Wang Weidong He Yuanfu Chen school of Electronic science and Engineering and State Key Laboratory of Electronic Thin Films and Integrated DevicesUniversity of Electronic Science and Technology of ChinaChengdu 610054PR China school of Physics University of Electronic Science and Technology of ChinaChengdu 611731PR China school of science and Institute of Oxygen SupplyTibet UniversityLhasa 850000PR China College of Materials science and Engineering Sichuan UniversityChengdu 610065PR China

The shuttle effect of lithium polysulfides(liPss)and sluggish redox conversion significantly hinder practical implementation of lithium-sulfur batteries(LsBs).To overcome these issues,herein,we present MoP quantum dots anchored N,P-doped graphene(MPQ@G)as a multifunctional LsB cathode.The N,P-doped graphene layers serve as a conductive skeleton to support the MoP QDs which can accelerate the electron transfer,physically hinder the polysulfide migration and thus enhance the electrochemical performance.More importantly,as a polar and conductive catalyst,MoP QDs provide catalytically active sites for the conversion of liPss.As a result,the LsBs with MPQ@G/s cathodes deliver an elevated initial capacity of 1220.2 mAh g~(-1)at 0.2 C and remain 98.9%after rate cycles,signifying its exceptional cycling stability.Moreover,it displays a large capacity of 681.2 mAh g~(-1)even at a high rate of 1 C.The li-s pouch cell also presents high specific capacities and preeminent cycling stabilities,confirming its great potential for high-rate applications.Density functional theory calculations demonstrate the improved absorptivity and redox conversion reversibility of liPss.This work provides an efficient strategy to improve composite with highly adsorptive and catalytic properties for high-performance li-s batteries.

关键词： MoP quantum dots Graphene Electrocatalyst shuttle effect li-s batteries

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Iron atom-nanoparticles for interactional enhancing the electrocatalytic reaction activity in li-s batteries

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Chinese Chemical Letters 2023年第11期34卷 311-316页

作者： Gamal H.Al-shawesh Jiawen Zhu Wei Zhang shuai Xie Junjie Xu Guolei Cai Amar Y.Al-Ansi Yunhong Wei song Jin Hengxing Ji Hefei National Laboratory for Physical sciences at the Microscale CAS Key Laboratory of Materials for Energy ConversionDepartment of Applied ChemistryUniversity of Science and Technology of ChinaHefei 230026China Department of Chemistry Faculty of EducationThamar UniversityDhamarYemen school of Chemistry and Chemical Engineering Hefei University of TechnologyHefei 230009China

The undesirable shuttle effect and sluggish redox kinetics of polysulfides seriously result in low sulfur utilization and poor capacity retention.Here,an integrated strategy is proposed by rational designing multifunctional architecture to manipulate the redox kinetics of polysulfides,specifically,by employing iron atoms(Fe-As)and iron-species nanoparticles(Fe-NPs)co-embedded nitrogen-doped carbon nanotube(Fe-NCNT)as catalyst and host for sulfur.The synergistic cooperation of Fe-As and Fe-NPs provides efficient active sites to facilitate the diffusion,strengthen the affinities,and promote the conversion reactions for polysulfides.Furthermore,the NCNT not only offers practical li+transport pathways but also immobilize the polysulfides effectively.Benefiting from these merits,the Fe-NCNT/s electrodes exhibit high initial specific capacity of 1502.6 mAh/g at 0.1 C,outstanding rate performance(830 mAh/g at 2 C),and good cycling performance(597.8 mAh/g after 500 cycles with an ultralow capacity fading rate of 0.069%per cycle).This work features the distinct interaction of iron atom-nanoparticles on facilitating immobilization-diffusion-transformation process of polysulfides,and it also expected to pave the way for the application in practical li-s batteries.

关键词： N-doped carbon nanotubes Iron atoms Iron nanoparticles Electrocatalyst li-s batteries

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Microwave-assisted synthesis of Cr_(3)C_(2)@C core shell structure anchored on hierarchical porous carbon foam for enhanced polysulfide adsorption in li-s batteries

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Nano Research 2021年第7期14卷 2345-2352页

作者： Xierong Zeng Jianxin Tu shuangshuang Chen shaozhong Zeng Qi Zhang Jizhao Zou Kezhi li shenzhen Key Laboratory of special Functional Materials&shenzhen Engineering Laboratory for Advance Technology of ceramics College of Materials Science and EngineeringShenzhen UniversityShenzhen 518060China state Key Laboratory of solidification Processing Carbon/Carbon Composites Research CenterNorthwestern Polytechnical UniversityXi’an 710072China school of Materials science and Engineering Anhui University of TechnologyMa'anshan 243002China College of New Materials and New Energies Shenzhen Technology UniversityShenzhen 518118China BCMaterials Basque Center for MaterialsApplications and NanostructuresUPV/EHU Science Park48940 LeioaSpainIKERBASQUEBasque Foundation for Science48013 BilbaoSpain

In this paper,we use microwave reduction strategy to synthesize a new bi-functional sulfur host material at the service of cathode substrate for lithium-sulfur batteries(LsBs),the composite is made of hierarchical porous carbon foam supported carbon-encapsulated chromium carbide nano-particles(Cr_(3)C_(2)@C/HPCF),in which the well-distributed conductive Cr_(3)C_(2) nano-particles can act as powerful chemical adsorbent and are effective in restraining the shuttle effect of lithium polysulfides(liPss).Test results show that the Cr_(3)C_(2)@C/HPCF based sulfur electrodes with 75 wt.%of sulfur exhibit a high initial discharging capacity of 1,321.1 mAh·g^(−1) at 0.1 C(3.5 mg·cm^(−2)),and a reversible capacity can still maintain stability at 1,002.1 mAh·g^(−1) after 150 cycles.Even increasing the areal sulfur loading to 4 mg·cm^(−2),the electrodes can still deliver an initial discharging capacity of 948.0 mAh·g^(−1) at 0.5 C with ultra-slow capacity decay rate of 0.075%per cycle during 500 cycles.Furthermore,the adsorption energy between the Cr_(3)C_(2) surface and liPss as well as theoretic analysis based on first-principles is also investigated.

关键词： Cr_(3)C_(2)nanoparticles core shell structure chemisorptions microwave reduction hierarchical porous carbon foam li-s batteries

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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

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Three-dimensional architectures based on carbon nanotube bridged Ti_(2)C MXene nanosheets for li-s batteries

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Particuology 2021年第4期19卷 139-145页

作者： Qinhua Gu Ming Lu Junnan Chen Yujie Qi Bingsen Zhang shenyang National Laboratory for Materials science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016China school of Materials science and Engineering University of Science and Technology of ChinaShenyang 110016China Key Laboratory of Functional Materials Physics and Chemistry of the Ministry of Education Jilin Normal UniversityChangchun 130103China

lithium-sulfur(li-s)batteries are promising candidates for high density electrochemical energy storage systems.However,the poor conductivity of s and the shuttle effect of polysulfides are a bottleneck to practical applications.Herein,a three-dimensional architecture,based on carbon nanotube(CNT)bridged Ti_(2)C MXene nanosheets,was constructed as a sulfur host.This architecture was based on Ti atoms,which can chemically absorb polysulfides.The CNTs are highly conductive and intercalate into the MXene nanosheets to prevent their stacking and construct an interspace for polysulfides.This hybrid,as a host of s,can effectively alleviate the shuttle effect through a combination of physical confinement and chemical adsorption.This resulted in an open internal space,which served as a cathode for the loaded s to promote electron transport and enhance electrochemical kinetics of the polysulfide conversion in li-s batteries.

关键词： li-s batteries shuttle effect MXene Polysulfides Three-dimensional(3D)architecture

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Designing Electrochemical Nanoreactors to Accelerate li_(2)s_(1/2) Three-Dimensional Growth Process and Generating More li_(2)s for Advanced li–s batteries

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Renewables 2023年第3期1卷 341-352页

作者： Junhao li Kaixiang shi Jiajie Pan Junda Pan Yongxian lin Kaixin Wang Hao li Jinyun liao Huafeng Dong Quanbing liu Guangzhou Key Laboratory of Clean Transportation Energy Chemistry Guangdong Provincial Key Laboratory of Plant Resources BiorefinerySchool of Chemical Engineering and Light IndustryGuangdong University of TechnologyGuangzhou 510006 Jieyang Branch of Chemistry and Chemical Engineering Guangdong Laboratory(Rongjiang Laboratory) Jieyang 515200 school of Chemistry and Materials Engineering Huizhou UniversityHuizhou516007 school of Physics and Optoelectronic Engineering Guangdong University of TechnologyGuangzhou 510006

With advantages of low costs and high energy density,li–s batteries are considered as one of the most promising energy storage devices.However,li_(2)s_(2) with a high dissociation energy and insulative properties is hard to convert into li_(2)s,resulting in underutilization of sulfur capacity.Herein,Co-Mo_(2)C@C yolk–shell spheres as nanoreactors were designed to confront this challenge rationally.The Co-Mo_(2)C@C-induced li_(2)s_(1/2) nucleation and growth in the three-dimensional process and the cathode produced more li_(2)s after full discharge.Experimental studies and theoretical calculations reveal that the conversion barrier from li_(2)s_(2) into li_(2)s was lowered while the diffusion of lithium ions and electron transfer accelerated when using the Co-Mo_(2)C@C catalyst.Based on the above advantages,the Co-Mo_(2)C@C/s cathode exhibits a high reversible capacity and excellent cyclic stability,such as an initial specific capacity of 1200 mAh g^(−1) at 0.1 C with 709 mAh g^(−1) at 1.0 C after 1000 cycles with a low capacity fading rate of 0.04%per cycle.Even at high densities of 3.0 C and 5.0 C,the specific capacities are 647.6 and 557.7 mAh g^(−1) after 400 cycles,respectively.Impressively,it also shows ca.770 and 900 mAh g^(−1) at 0.2 C after 50 cycles with high sulfur loadings of 4.2 and 5.1 mg cm−2,respectively.The present work may provide new insights into the design of nanoreactors to promote li_(2)s_(1/2) growth in a three-dimensional process and accelerate conversion from solid li_(2)s_(2) to solid li_(2)s in high performance li–s batteries.

关键词： li-s batteries cobalt-dopedβ-Mo_(2)C yolk-shell structure optimizing li_(2)s_(1/2)growth process fast solid-solid conversion of li_(2)s_(2)-li_(2)s

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Graphene-Based sulfur Composites for Energy storage and Conversion in li-s batteries

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Chinese Journal of Chemistry 2016年第1期34卷 13-31页

作者： Xingxing Gu shanqing Zhang Yanglong Hou Department of Materials science and Engineering College of Engineering Peking University Beijing 100871 China Centre for Clean Environment and Energy Environmental Futures Insititute Griffith School of Environment Gold Coast Campus Griffith University QLD 4222 Australia

There are growing research interests in developing high-performance energy storage systems to meet the demands for large-scale and sustainable energy storage. The lithium-sulfur （li-s） batteries have drawn numerous attentions due to their exceptionally high energy density compared with other batteries. However, achieving the high capacities with long-term cycle stability and retaining an essentially high sulfur loading remains a tremendous chal- lenge for the designs of li-s batteries. Graphene is regarded as a very suitable and promising addition to the com- positions for li-s batteries due to its unique two dimensional （2D） structure, high conductivity and superior me- chanical flexibility. Besides, the functional groups of graphene surface can be tuned flexibly to immobilize the s/li2sx on the graphene surface during the cycling process. In this review, the development of graphene-sulfur composites and their applications in li-s batteries are discussed. The attempts are also devoted to the synthesis approaches of various graphene-based sulfur composites, the graphene-sulfur interaction and the impacts on the elec- trochemical performances as well as the major issues of li-s batteries.

关键词： li-s batteries graphene-sulfur composites polysulfides immobilization

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