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Catalyzing the polysulfide conversion for promoting lithium sulfur battery performances:A review

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Journal of Energy Chemistry 2021年第3期30卷 434-451页

作者： Jingfa Li Zhihao Niu Cong Guo Min Li Weizhai Bao School of Chemistry and Materials Science Nanjing University of Information Science and TechnologyNanjing 210044JiangsuChina Jiangsu Key Laboratory for Optoelectronic Detection of Atmosphere and Ocean School of Physics and Optoelectronic EngineeringNanjing University of Information Science and TechnologyNanjing 210044JiangsuChina

Lithium-sulfur batteries(LSBs)are being recognized as potential successor to ubiquitous LIBs in daily life due to their higher theoretical energy density and lower cost effectiveness.However,the development of the LSB is beset with some tenacious issues,mainly including the insulation nature of the S or Li_(2)S(the discharged product),the unavoidable dissolution of the reaction intermediate products(mainly as lithium polysulfides(LiPSs)),and the subsequent LiPSs shuttling across the separator,resulting in the continuous loss of active material,anode passivation,and low coulombic efficiency.Containment methods by introducing the high-electrical conductivity host are commonly used in improving the electrochemical performances of LSBs.However,such prevalent technologies are in the price of reduced energy density since they require more addition of amount of host materials.Adding trace of catalysts that catalyze the redox reaction between S/Li_(2)S and Li_(2)Sn(3conversion reaction between the solid S species and dissolved S species,alleviating the shuttle effect,but also expedites the electron transport thus reducing the polarization of the electrode.In this review,the redox reaction process during Li-S chemistry are firstly highlighted.Recent developed catalysts,including transitionmetal oxides,chalcogenides,phosphides,nitrides,and carbides/borides are then outlined to better understand the role of catalyst additives during the polysulfide conversion.Finally,the critical issues,challenges,and perspectives are discussed to demonstrate the potential development of LSBs.

关键词： Catalyst Kinetics Shuttle effect polysulfide conversion Lithium sulfur battery

polysulfide regulation by defect-modulated Ta_(3)N_(5-x) electrocatalyst toward superior room-temperature sodium-sulfur batteries

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Science Bulletin 2024年第2期69卷 197-208页

作者： Zhen Zhang Dan Luo Jun Chen Chuyin Ma Matthew Li Haoze Zhang Renfei Feng Rui Gao Haozhen Dou Aiping Yu Xin Wang Zhongwei Chen Department of Chemical Engineering Waterloo Institute for NanotechnologyUniversity of WaterlooWaterloo N2L 3G1Canada Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023China South China Academy of Advanced Optoelectronics&International Academy of Optoelectronics at Zhaoqing South China Normal UniversityGuangzhou 510006China Chemical Sciences and Engineering Division Argonne National LaboratoryLemont 60439USA Canadian Light Source Saskatoon S7N 2V3Canada

Resolving low sulfur reaction activity and severe polysulfide dissolution remains challenging in metalsulfur batteries.Motivated by a theoretical prediction,herein,we strategically propose nitrogenvacancy tantalum nitride(Ta3N5-x)impregnated inside the interconnected nanopores of nitrogendecorated carbon matrix as a new electrocatalyst for regulating sulfur redox reactions in roomtemperature sodium-sulfur batteries.Through a pore-constriction mechanism,the nitrogen vacancies are controllably constructed during the nucleation of Ta3N5-x.The defect manipulation on the local environment enables well-regulated Ta 5d-orbital energy level,not only modulating band structure toward enhanced intrinsic conductivity of Ta-based materials,but also promoting polysulfide stabilization and achieving bifunctional catalytic capability toward completely reversible polysulfide conversion.Moreover,the interconnected continuous Ta3N5-x-in-pore structure facilitates electron and sodium-ion transport and accommodates volume expansion of sulfur species while suppressing their shuttle behavior.Due to these attributes,the as-developed Ta3N5-x-based electrode achieves superior rate capability of 730 mAh g-1 at 3.35 A g-1,long-term cycling stability over 2000 cycles,and high areal capacity over 6 mAh cm-2 under high sulfur loading of 6.2 mg cm-2.This work not only presents a new sulfur electrocatalyst candidate for metal-sulfur batteries,but also sheds light on the controllable material design of defect structure in hopes of inspiring new ideas and directions for future research.

关键词： Tantalum nitride Nitrogen defects Sodium-sulfur batteries Electrocatalysts polysulfide conversion

Carbon-Nitride-Based Materials for Advanced Lithium-Sulfur Batteries

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Nano-Micro Letters 2022年第12期14卷 579-601页

作者： Wenhao Sun Zihao Song Zhenxing Feng Yaqin Huang Zhichuan J.Xu Yi-Chun Lu Qingli Zou State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029People’s Republic of China Electrochemical Energy and Interfaces Laboratory Department of Mechanical and Automation EngineeringThe Chinese University of Hong KongHong Kong Special Administrative Region 999077People’s Republic of China School of Materials Science and Engineering Nanyang Technological UniversitySingapore 639798Republic of Singapore School of Chemical Biologicaland Environmental EngineeringOregon State UniversityCorvallisOR 97331USA

Lithium-sulfur(Li-S)batteries are promising candidates for next-generation energy storage systems owing to their high energy density and low cost.However,critical challenges including severe shuttling of lithium polysulfides(LiPSs)and sluggish redox kinetics limit the practical application of Li-S batteries.Carbon nitrides(C_(x)N_(y)),represented by graphitic carbon nitride(g-C_(3)N_(4)),provide new opportunities for overcoming these challenges.With a graphene-like structure and high pyridinic-N content,g-C_(3)N_(4) can effectively immobilize LiPSs and enhance the redox kinetics of S species.In addition,its structure and properties including electronic conductivity and catalytic activity can be regulated by simple methods that facilitate its application in Li-S batteries.Here,the recent progress of applying C_(x)N_(y)-based materials including the optimized g-C_(3)N_(4),g-C_(3)N_(4)-based composites,and other novel C_(x)N_(y) materials is systematically reviewed in Li-S batteries,with a focus on the structure-activity relationship.The limitations of existing C_(x)N_(y)-based materials are identified,and the perspectives on the rational design of advanced C_(x)N_(y)-based materials are provided for high-performance Li-S batteries.

关键词： Lithium-sulfur batteries Carbon nitride polysulfide conversion Shuttle effect Anode protection

Synthesis and application of single-atom catalysts in sulfur cathode for high-performance lithium–sulfur batteries

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Chinese Chemical Letters 2023年第1期34卷 73-83页

作者： Yingjie Miao Yufan Zheng Feng Tao Zhijun Chen Yi Xiong Fengzhang Ren Yong Liu Provincial and Ministerial Co-Construction of Collaborative Innovation Center for Non-Ferrous Metal New Materials and Advanced Processing Technology Henan Key Laboratory of Non-Ferrous Materials Science and Processing TechnologySchool of Materials Science and EngineeringHenan University of Science and TechnologyLuoyang 471023China School of Intelligent Manufacturing Ecosystem Xi’an Jiaotong–Liverpool UniversitySuzhou 215123China Luoyang Bearing Research Institute Co. Ltd.Luoyang 471039China

Lithium–sulfur(Li-S)batteries are regarded as one of the most promising energy storage devices because of their low cost,high energy density,and environmental friendliness.However,Li-S batteries suffer from sluggish reaction kinetics and serious“shuttle effect”of lithium polysulfides(LiPSs),which causes rapid decay of battery capacity and prevent their practical application.To address these problems,introducing single-atom catalysts(SACs)is an effective method to improve the electrochemical performance of Li-S batteries,due to their high catalytic efficiency and definite active sites for LiPSs.In this paper,we summarized the latest developments in enhancing the electrochemical performance of cathode for Li-S batteries through introducing different SACs.Furthermore,we briefly introduced the catalytic mechanism of SACs and discussed the strategies of synthesizing SACs,including the spatial confinement strategy and the coordination design strategy.Finally,the challenges and prospects in this field are proposed.We believe that this review would help to design and fabricate high-performance Li-S batteries via introducing SACs and boost their practical application.

关键词： Single-atom catalysts Lithium-sulfur batteries Sulfur cathode Synthesis and application polysulfide conversion Shuttle effect

High-density oxygen-doped nano-TaN enables robust polysulfide interconversion in Li−S batteries

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中国化学快报:英文版 2023年第8期34卷 360-364页

作者： Shuang Yu Yonggui Zhang Shuo Yang Kuikui Xiao Dong Cai Huagui Nie Zhi Yang Key Laboratory of Carbon Materials of Zhejiang Province Wenzhou UniversityWenzhou 325035China College of Electrical and Electronic Engineering Wenzhou UniversityWenzhou 325035China

To tackle undesirable shuttle reaction and sluggish reaction kinetics in lithium–sulfur(Li–S)batteries,we develop a porous and high-density oxygen-doped tantalum nitride nanostructure(nano-TaNO)as an efficient catalyst through delicate tailoring.Benefiting from well-defined interior and surface nanopore channels,the nano-TaNO favors abundant sulfur storage,easy electrolyte infiltration and good electrons/Li+transport.More importantly,high-density O dopant in nano-TaNO not only provides high conductivity,but also promotes polysulfide adsorption/conversion via Li–O chemical interactions and the generation of S3∗−radicals to activate additional evolution path from S8 to Li_(2)S.Consequently,the nano-TaNObased cathode exhibits excellent specific capacity and cyclability even under high sulfur loading condition.These interesting findings suggest the great potential of tantalum nitride and a high amount of anion doping engineering in manipulating intermediates and building high-performance Li−S rechargeable batteries.

关键词： Lithium−sulfur batteries polysulfide conversion O doping TaN High-density

High-Entropy Spinel Oxide Nanofibers as Catalytic Sulfur Hosts Promise the High Gravimetric and Volumetric Capacities for Lithium–Sulfur Batteries

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Energy & Environmental Materials 2022年第2期5卷 645-654页

作者： Liyuan Tian Ze Zhang Sheng Liu Guoran Li Xueping Gao Institute of New Energy Material Chemistry School of Materials Science and EngineeringRenewable Energy Conversion and Storage CenterNankai UniversityTianjin 300350China

The exploration of new catalytic hosts is highly important to tackle the sluggish electrochemical kinetics of sulfur redox for achieving high energy density of lithium–sulfur batteries.Herein,for the first time,we present high-entropy oxide(HEO,(Mg_(0.2)Mn_(0.2)Ni_(0.2)Co_(0.2)Zn_(0.2))Fe_(2)O_(4))nanofibers as catalytic host of sulfur.The HEO nanofibers show a synergistic effect among multiple metal cations in spinel structure that enables strong chemical confinement of soluble polysulfides and fast kinetics for polysulfide conversion.Consequently,the S/HEO composite displays the high gravimetric capacity of 1368.7 mAh g^(−1) at 0.1 C rate,excellent rate capability with the discharge capacity of 632.1 mAh g^(−1) at 5 C rate,and desirable cycle stability.Furthermore,the S/HEO composite shows desirable sulfur utilization and good cycle stability under a harsh operating condition of high sulfur loading(4.6 mg cm^(−2))or low electrolyte/sulfur ratio(5μL mg^(−1)).More impressively,the high volumetric capacity of 2627.9 mAh cm^(−3) is achieved simultaneously for the S/HEO composite due to the high tap density of 1.92 g cm^(−3),nearly 2.5 times of the conventional sulfur/carbon composite.Therefore,based on high-entropy oxide materials,this work affords a fresh concept of elevating the gravimetric/volumetric capacities of sulfur cathodes for lithium–sulfur batteries.

关键词： catalytic host high-entropy oxide lithium-sulfur battery polysulfide conversion spinel oxide nanofibers

Single-atom catalysis enables long-life, high-energy lithium-sulfur batteries

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Nano Research 2020年第7期13卷 1856-1866页

作者： Zechao Zhuang Qi Kang Dingsheng Wang Yadong Li Department of Chemistry Tsinghua UniversityBeijing 100084China Department of Polymer Science and Engineering Shanghai Key Laboratory of Electrical Insulation and Thermal AgeingShanghai Jiao Tong UniversityShanghai 200240China

With high energy density and low material cost,lithium sulfur batteries(LSBs)emerge quite expeditiously as a fascinating energy storage system over the past decade.Broad applications of LSBs ranging from electric vehicles to stationary grid storage seem rather bright in recent literatures.However,there still exist many pressing challenges to be addressed because we do not yet fully understand and control the electrode-electrolyte interface chemistries during battery operation,such as polysulide shuttling and poor utilization of active sulfur.Single-atom catalysts(SACs)pave new possibilities of tackling the tough issues due to their decent applicability in the atomic-level identification of structure-activity relationships and reaction mechanism,as well as their structural tunability with atomic precision.This review comprehensively summarizes the very recent advances in utilization of highly active SACs for LSBs by stating and discussing the related publications,which involves catalyst synthesis routes,battery pertormance,catalytic mechanisms,optimization strategies,and promises to achieve long-lite,high-energy LSBs.We see that endeavors to employ SACs to modify sulfur cathode have allowed efficient polysulfide conversion and confinement,leading to the minimization of shuttle effect.Parallel efforts are being devoted to extending the scope of SACs to cell separator and lithium metal anode in order to unlock the full potential of LSBs.We also obtain mechanistic insights into battery chemistries and nature of SACs in their strong interactions with polysulfides through advanced in situ characterizations documented.Overall,acceleration in the development of LSBs by introducing SACs is noticeable,and this cutting edge needs more attentions to further promoting the design of better LSBs.

关键词： single-atom catalysis lithium-sulfur battery polysulfide conversion shuttle effect atomic-level insight

Cooperative catalytic platinum species accelerating polysulfide redox reactions for Li-S batteries

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Journal of Energy Chemistry 2023年第12期87卷 123-135,I0005页

作者： Yujie Qi Ning Chai Qinhua Gu Junnan Chen Zhaofeng Zhai Ming Lu Yiming Niu Nan Huang Xia Zhang Bingsen Zhang Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016LiaoningChina School of Materials Science and Engineering University of Science and Technology of ChinaShenyang 110016LiaoningChina Department of Chemistry College of ScienceNortheastern UniversityShenyang 110819LiaoningChina The Joint Laboratory of MXene Materials Key Laboratory of Functional Materials Physics and Chemistry of the Ministry of EducationKey Laboratory of Preparation and Application of Environmental Friendly Materials of the Ministry of EducationJilin Normal UniversityChangchun 130103JilinChina

The shuttle effect derived from diffusion of lithium polysulfides(LiPSs) and sluggish redox kinetic bring about poor cycling stability and low utilization of sulfur,which have always been the key challenging issues for the commercial application of lithium-sulfur(Li-S) batteries.Rational design of cathode materials to catalyze Li_(2)S dissociation/nucleation processes is an appealing and valid strategy to develop high-energy practical Li-S batteries.Herein,considering the synergistic effect of bidirectional catalysis on LiPSs conversion and enhanced chemical immobilization for LiPSs by heteroatom doping,Pt nanoparticles loaded on nitrogen-doped carbon spheres(Pt/NCS composites) were constructed as cathode materials.According to the dynamic evolution of Pt catalysts and sulfur species,Pt~0 and Pt^(2+) species were identified as active species for the accelerated dissociation and nucleation of Li_(2)S,respectively.Meanwhile,in-situ Raman results demonstrated the expedited conversion of sulfur species resulted from bidirectional catalysis of active Pt species,corresponding to boosted redox kinetics.Consequently,Pt/NCS cathode exhibited improved long-term cyclability with high initial capacity,along with enhanced rate capability.This work provides a facile approach to construct cathode materials with bidirectional catalysis on Li_(2)S dissociation/nucleation,and sheds light on a more global understanding of the catalytic mechanism of metal catalysts during LiPSs conversion.

关键词： Lithium-sulfur batteries Platinum species N-doped carbon spheres Bidirectional catalysis polysulfide conversion