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Engineering hollow core-shell hetero-structure box to induce interfacial charge modulation for promoting bidirectional sulfur conversion in lithium-sulfur batteries

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Journal of Energy Chemistry 2023年第5期80卷 128-139,I0004页

作者： Weiliang Zhou Xinying Wang Jiongwei Shan Liguo Yue Dongzhen Lu Li Chen Jiacheng Zhang Yunyong Li School of Materials and Energy Guangdong University of TechnologyNo.100 Waihuan Xi RoadGuangzhou Higher Education Mega CenterGuangzhou 510006GuangdongChina

Severe polysulfide shuttling and sluggish sulfur redox kinetics significantly decrease sulfur utilization and cycling stability in lithium-sulfur batteries(LSBs).Herein,we develop a hollow CoO/CoP-Box core-shell heterostructure as a model and multifunctional catalyst modified on separators to induce interfacial charge modulation and expose more active sites for promoting the adsorption and catalytic conversion ability of sulfur species.Theoretical and experimental findings verify that the in-situ formed core-shell hetero-interface induces the formation of P-Co-O binding and charge redistribution to activate surface O active sites for binding lithium polysulfides(LiPSs)via strong Li-O bonding,thus strongly adsorbing with Li PSs.Meanwhile,the strong Li-O bonding weakens the competing Li-S bonding in LiPSs or Li2S adsorbed on CoO/CoP-Box surface,plus the hollow heterostructure provides abundant active sites and fast electron/Li+transfer,so reducing Li2S nucleation/dissolution activation energy.As expected,LSBs with CoO/CoP-Box modified separator and traditional sulfur/carbon black cathode display a large initial capacity of 1240 mA h g^(-1)and a long cycling stability with 300 cycles(~60.1%capacity retention)at 0.5C.Impressively,the thick sulfur cathode(sulfur loading:5.2 mg cm^(-2))displays a high initial areal capacity of 6.9 mA h cm^(-2).This work verifies a deep mechanism understanding and an effective strategy to induce interfacial charge modulation and enhance active sites for designing efficient dual-directional Li-S catalysts via engineering hollow core-shell hetero-structure.

关键词： CoO/CoP-Box Hollow core-shell hetero-structure Multifunctional catalysts Interfacial charge modulation lithium sulfur batteries

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Toward high-sulfur-content,high-performance lithium-sulfur batteries:Review of materials and technologies

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Journal of Energy Chemistry 2023年第5期80卷 625-657,I0014页

作者： Fulai Zhao Jinhong Xue Wei Shao Hui Yu Wei Huang Jian Xiao School of Materials Science and Engineering Tianjin UniversityTianjin 300072China Basic Department Jinci College of Shanxi Medical UniversityTaiyuan 030025ShanxiChina School of Engineering Westlake UniversityHangzhou 310024ZhejiangChina School of Physics and Electronic Information Shangrao Normal UniversityShangrao 334001JiangxiChina

lithium sulfur batteries(LSBs)are recognized as promising devices for developing next-generation energy storage systems.In addition,they are attractive rechargeable battery systems for replacing lithium-ion batteries(LIBs)for commercial use owing to their higher theoretical energy density and lower cost compared to those of LIBs.However,LSBs are still beset with some persistent issues that prevent them from being used industrially,such as the unavoidable dissolution of lithium polysulfide intermediates during electrochemical reactions and large volume expansion(up to 80%)upon the formation of Li_(2)S,resulting in serious battery life and safety limitations.In the process of solving these problems,it is necessary to maintain a high sulfur content in the cathode materials to ensure that the LSBs have high energy densities and excellent cycle performance.In this review,the novel preparation methods and cathode materials used for preparing LSBs in recent years are reviewed considering the sulfur content and cycle performance.In addition,the problems and difficulties in practically applying cathode materials are described,and the development trend is discussed.

关键词： lithium sulfur batteries Cathode material High sulfur content Cycle performance

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Facile synthesis of sulfurized polyacrylonitrile composite as cathode for high-rate lithium-sulfur batteries

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Journal of Energy Chemistry 2020年第10期29卷 161-165页

作者： Jingwei Xiang Zezhou Guo Ziqi Yi Yi Zhang Lixia Yuan Zexiao Cheng Yue Shen Yunhui Huang State Key Laboratory of Material Processing and Die&Mold Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiChina

sulfurized polyacrylonitrile(SPAN)as a promising cathode material for lithium sulfur(Li-S)batteries has drawn increasing attention for its improved electrochemical performance in carbonate-based electrolyte.However,the relatively poor electronic and ionic conductivities of SPAN limit its high-rate and lowtemperature performances.In this work,a novel one-dimensional nanofiber SPAN(SFPAN)composite is developed as the cathode material for Li-S batteries.Benefitting from its one-dimensional nanostructure,the SFPAN composite cathode provides fast channels for the migration of ions and electronics,thus effectively improving its electrochemical performance at high rates and low temperature.As a result,the SFPAN maintains a high reversible specific capacity^1200 mAh g−1 after 400 cycles at 0.3 A g−1 and can deliver a high capacity of^850 mAh g−1 even at a high current density of 12.5 A g−1.What is more,the SFPAN can achieve a capacity of^800 mAh g−1 at 0℃and^1550 mAh g−1 at 60℃,thus providing a wider temperature range of applications.This work provides new perspectives on the cathode design for high-rate lithium-sulfur batteries.

关键词： sulfurized polyacrylonitrile One-dimensional nanofiber High-rate peformance lithium sulfur batteries

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FeCo alloy catalysts promoting polysulfide conversion for advanced lithium-sulfur batteries

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Journal of Energy Chemistry 2020年第10期29卷 339-347页

作者： Hongyi Li Linfeng Fei Rong Zhang Shenglan Yu Yongyi Zhang Longlong Shu Yong Li Yu Wang School of Materials Science and Engineering Nanchang UniversityNanchang 330031JiangxiChina Division of Nanomaterials and Jiangxi Key Lab of Carbonene Materials Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesNanchang 330200JiangxiChina College of Chemistry Biology and Material ScienceEast China University of TechnologyNanchang 330013JiangxiChina

lithium sulfur batteries(LSBs)draw extensive interest because of the ultra-high capacity and low material cost.However,the sluggish lithium polysulfides(LIPSs)conversion processes are detrimental to cycle stability and rate capability,inhibiting the commercial application of LSBs.Here we present the well-designed Fe Co alloy catalysts anchored on porous carbon(FeCo-C)as sulfur host to improve the electrochemical performance by accelerating the conversion reactions.The FeCo alloy demonstrates high catalytic effect and strong adsorption capability of LIPSs,in which potential polarization can be greatly decreased and"shuttle effects"can be largely avoided.As a result,the obtained S/Fe Co-C composites show an initial specific capacity of 791.9 m Ah g^-1 at a large current density of 2 C and maintain 502.5 mAh g^-1 even after 500 cycles.Moreover,720 m Ah g^-1(corresponding to 70%retention)can be achieved after 100 cycles at 0.2 C with a high sulfur content of 80 wt%,enabling high sulfur utilization.This work not only provides a new insight to investigate the conversion kinetics of Li PSs,but also opens up a new avenue for advanced lithium sulfur batteries.

关键词： lithium sulfur batteries FeCo alloys Catalysts Adsorption Porous carbon

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Revealing the working mechanism of a multi-functional block copolymer binder for lithium-sulfur batteries

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Journal of Energy Chemistry 2021年第8期30卷 1-8,I0001页

作者： Xin He Zhimeng Liu Guoping Gao Xiaotao Liu Michal Swietoslawski Jun Feng Gao Liu Lin-Wang Wang Robert Kostecki Energy Storage&Distributed Resources Division Lawrence Berkeley National Laboratory1 Cyclotron Road94720 BerkeleyUSA Materials Sciences Division Lawrence Berkeley National Laboratory94720 BerkeleyUSA The Molecular Foundry Lawrence Berkeley National Laboratory94720 BerkeleyUSA Department of Materials Science&Engineering Southern University of Science and Technology(SUSTech)Shenzhen 518055China

The lithium-sulfur(Li-S)battery is one of the most promising substitutes for current energy storage systems because of its low cost,high theoretical capacity,and high energy density.However,the high solubility of intermediate products(i.e.,lithium polysulfides)and the resultant shuttle effect lead to rapidly fading capacity and a low coulombic efficiency,which hinder the practical application of Li-S batteries.In this study,block copolymers are constructed with both an ethylene oxide unit and a styrene unit and then used as binders for Li-S batteries.Electrochemical performance improvements are attributed to the synergistic effects contributed by the different units of the block copolymer.The ethylene oxide unit traps polysulfide,which bonds strongly with the intermediate lithium polysulfide,and enhances the transport of lithium ions to reach high capacity.Meanwhile,the styrene unit maintains cathode integrity by improving the mechanical properties and elasticity of the constructed block copolymer to accommodate the large volume changes.By enabling multiple functions via different units in the polymer chain,high sulfur utilization is achieved,polysulfide diffusion is confined,and the shuttle effect is suppressed during the cycle life of Li-S batteries,as revealed by operando ultraviolet-visible spectroscopy and S Kedge X-ray absorption spectroscopy.

关键词： lithium sulfur batteries Polymer binder Block copolymer Ultraviolet-visible spectroscopy X-ray absorption spectroscopy

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Deciphering pitting behavior of lithium metal anodes in lithium sulfur batteries

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Journal of Energy Chemistry 2020年第10期29卷 257-261页

作者： Fanyang Huang Shuai Wang Yulin Jie Evan Hansen Shiyang Wang Zhanwu Lei Jian Liu Ruiguo Cao Genqiang Zhang Shuhong Jiao 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 230026AnhuiChina School of Engineering Faculty of Applied ScienceUniversity of British ColumbiaKelownaBCV1V1V7Canada

Unambiguous understanding in lithium anode failure mechanism calls for a comprehensive methodology to investigate the coupled morphological,electrochemical and mechanical behaviors during the stripping process.In this work,a mechanistic investigation of the pitting behavior of lithium metal in an electrolyte containing lithium polysulfides in lithium sulfur batteries was developed.It is found that lithium polysulfides could aggravate the nonuniform stripping of lithium electrodes.

关键词： lithium anode Pitting behavior Failure mechanism lithium sulfur batteries

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Edge sulfurized graphene nanoplatelets via vacuum mechano-chemical reaction for lithium–sulfur batteries

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Journal of Energy Chemistry 2017年第3期26卷 522-529页

作者： Longlong Yan Min Xiao Shuanjin Wang Dongmei Han Yuezhong Meng The Key Laboratory of Low-Carbon Chemistry&Energy Conservation of Guangdong Province/State Key Laboratory of Optoelectronic Materials and Technologies School of Materials Science and EngineeringSun Yat-sen UniversityGuangzhou 510275GuangdongChina Sino-French Institute of Nuclear Engineering and Technology Sun Yat-sen UniversityZhuhai 519082GuangdongChina

lithium–sulfur batteries have great potential for high energy applications due to their high capacities,low cost and eco-friendliness. However, the particularly rapid capacity decay owing to the dissolution and diffusion of polysulfide intermediate into the electrolyte still hamper their practical applications.And the reported preparation procedures to sulfur based cathode materials are often complex, and hence are rather difficult to produce at large scale. Here, we report a simple mechano-chemical sulfurization methodology in vacuum environment applying ball-milling method combined both the chemical and physical interaction for the one-pot synthesis of edge-sulfurized grapheme nanoplatelets with 3D porous foam structure as cathode materials. The optimal sample of 70%S–Gn Ps-48 h(ball-milled 48 h) obtains 13.2 wt% sulfur that chemically bonded onto the edge of Gn Ps. And the assembled batteries exhibit high initial discharge capacities of 1089 mAh/g at 0.1 C and 950 mAh/g at 0.5 C, and retain a stable discharge capacity of 776 mAh/g after 250 cycles at 0.5 C with a high Coulombic efficiency of over 98%. The excellent performance is mainly attributed to the mechano-chemical interaction between sulfur and grapheme nanoplatelets. This definitely triggers the currently extensive research in lithium–sulfur battery area.

关键词： lithium sulfur batteries Graphene nanoplatelets Edge-functionalized with sulfur 3D porous foam structure Mechano-chemical interaction

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Towards full demonstration of high areal loading sulfur cathode in lithium–sulfur batteries

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Journal of Energy Chemistry 2019年第12期28卷 17-22页

作者： Long Kong Qi Jin Xi-Tian Zhang Bo-Quan Li Jin-Xiu Chen Wan-Cheng Zhu Jia-Qi Huang Qiang Zhang Beijing Key Laboratory o f Green Chemical Reaction Engineering and Technology Department of Chemical Engineering Tsinghua UniversityBeijing 100084China Key Laboratory for Photonic and Electronic Bandgap Materials Ministry of EducationSchool of Physics and Electronic EngineeringHarbin Normal UniversityHarbin 150025HeilongjiangChina Department of Chemical Engineering Qufu Normal UniversityQufu 273165ShandongChina Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China

lithium–sulfur(Li–S)batteries have been recognized as promising substitutes for current energy-storage technologies owing to their exceptional advantages in very high-energy density and excellent material sustainability.The cathode with high sulfur areal loading is vital for the practical applications of Li–S batteries with very high energy density.However,the high sulfur loading in an electrode results in poor rate and cycling performances of batteries in most cases.Herein,we used diameters of 5.0(D5)and 13.0(D13)mm to probe the effect of electrodes with different sizes on the rate and cycling performances under a high sulfur loading(4.5 mg cm^-2).The cell with D5 sulfur cathode exhibits better rate and cycling performances comparing with a large(D13)cathode.Both the high concentration of lithium polysulfides and corrosion of lithium metal anode impede rapid kinetics of sulfur redox reactions,which results in inferior battery performance of the Li–S cell with large diameter cathode.This work highlights the importance of rational matching of the large sulfur cathode with a high areal sulfur loading,carbon modified separators,organic electrolyte,and Li metal anode in a pouch cell,wherein the sulfur redox kinetics and lithium metal protection should be carefully considered under the flooded lithium polysulfide conditions in a working Li–S battery.

关键词： lithium sulfur batteries High areal sulfur loading lithium anode protection sulfur redox reactions Polysulfide interm ediates

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Carbon-based flexible self-supporting cathode for lithium-sulfur batteries:Progress and perspective

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Carbon Energy 2021年第2期3卷 271-302页

作者： Qinghuiqiang Xiao Jinlin Yang Xiaodong Wang Yirui Deng Peng Han Ning Yuan Lei Zhang Ming Feng Chang‐an Wang Ruiping Liu Department of Materials Science and Engineering China University of Mining and Technology(Beijing)BeijingChina School of Materials Science and Engineering Tsinghua UniversityBeijingChina Department of Mechanical Engineering University of Alaska FairbanksFairbanksAlaskaUSA Department of Applied Physics Key Laboratory of Functional Materials Physics and Chemistry of the Ministry of EducationJilin Normal UniversityChangchunChina

The flexible self-supporting electrode can maintain good mechanical and electrical properties while retaining high specific capacity,which meets the requirements of flexible batteries.lithium-sulfur batteries(LSBs),as a new generation of energy storage system,hold much higher theoretical energy density than traditional batteries,and they have attracted extensive attention from both the academic and industrial communities.Selection of a proper substrate material is important for the flexible self-supporting electrode.Carbon materials,with the advantages of light weight,high conductivity,strong structural plasticity,and low cost,provide the electrode with a large loading space for the active material and a conductive network.This makes the carbon materials meet the mechanical and electrochemical requirements of flexible electrodes.In this paper,the commonly used fabrication methods and recent research progresses of the flexible self-supporting cathode with a carbon material as the substrate are introduced.Various sulfur loading methods are summarized,which provides useful information for the structural design of the cathode.As the first review article of the carbon-based flexible self-supporting LSB cathodes,it provides valuable guidance for the researchers working in the field of LSB.

关键词： carbon flexible lithium sulfur batteries self-supporting

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Carbon Encapsulated Nickel Nanocomposites for the Cathode in Advanced lithium sulfur batteries

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China Petroleum Processing & Petrochemical Technology 2021年第4期23卷 1-6页

作者： Yang Yuxiang Xie Jingxin Wu Genghuang Zhu Na Li Huan Rong Junfeng SINOPEC Research Institute of Petroleum Processing Beijing 100083

lithium sulfur(Li-S)batteries are poised to be the next generation of high-density energy storage devices.In recent years,the concept of“electrocatalysis”has been introduced into the field of Li-S batteries,and some transition metals have been proved to catalyze the electrochemical conversion reaction of sulfur species.In this study,carbon encapsulated nickel nanoparticles(Ni@C)with a specific surface area of 146 m^(2)/g are shown to play a definitive electrocatalytic role for the sulfur cathode.With Ni@C incorporated,the Ni@C/G-S electrode achieved a better electrochemical performance than the G-S electrode.Moreover,the reversible capacity and cycle stability were further improved through chemical modifications of the carbon shell.The influence of doping with different elements on the Li-S battery performance was also investigated in detail.Higher specific capacities of 1229 mA·h/g,927 mA·h/g,and 830 mA·h/g were achieved at 0.2 C,0.5 C,and 1.0 C for the N-Ni@C-G/S electrode.Besides,the B-Ni@C-G/S electrode possessed a best cycle stability.

关键词： lithium sulfur batteries electrocatalysis electrochemical conversion reaction Ni@C chemical modifications

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