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Current collectors based on multiwalled carbon-nanotubes and fewlayer graphene for enhancing the conversion process in scalable lithium-sulfur battery

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Nano Research 2023年第6期16卷 8433-8447页

作者： Vittorio Marangon Edoardo Barcaro Luca Minnetti Wolfgang Brehm Francesco Bonaccorso Vittorio Pellegrini Jusef Hassoun Graphene Labs Istituto Italiano di TecnologiaGenoa 16163Italy Department of Chemical Pharmaceutical and Agricultural SciencesUniversity of FerraraFerrara 44121Italy BeDimensional S.p.A. Genoa 16163Italy National Interuniversity Consortium of Materials Science and Technology(INSTM) University of Ferrara Research UnitFerrara 44121Italy

We investigated herein the morphological,structural,and electrochemical features of electrodes using a sulfur(S)-super P carbon(SPC)composite(i.e.,S@SPC-73),and including few-layer graphene(FLG),multiwalled carbon nanotubes(MWCNTs),or a mixture of them within the current collector design.Furthermore,we studied the effect of two different electron-conducting agents,that is,SPC and FLG,used in the slurry for the electrode preparation.The supports have high structural crystallinity,while their morphologies are dependent on the type of material used.Cyclic voltammetry(CV)shows a reversible and stable conversion reaction between Li and S with an activation process upon the first cycle leading to the decrease of cell polarization.This activation process is verified by electrochemical impedance spectroscopy(EIS)with a decrease of the resistance after the first CV scan.Furthermore,CV at increasing scan rates indicates a Li+diffusion coefficient(D)ranging between 10^(−9) and 10^(−7) cm^(2)·s^(−1)in the various states of charge of the cell,and the highest D value for the electrodes using FLG as electron-conducting agent.Galvanostatic tests performed at constant current of C/5(1 C=1675 mA·g_(s)^(−1))show high initial specific capacity values,which decrease during the initial cycles due to a partial loss of the active material,and subsequently increase due to the activation process.All the electrodes show a Coulombic efficiency higher than 97%upon the initial cycles,and a retention strongly dependent on the electrode formulation.Therefore,this study suggests a careful control of the electrode in terms of current collector design and slurry composition to achieve good electrode morphology,mechanical stability,and promising electrochemical performance in practical Li-S cells.

关键词： lithium-sulfur battery current collector few-layer graphene carbon nanotubes scalability sulfur loading

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Characteristics of a gold-doped electrode for application in high-performance lithium-sulfur battery

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Journal of Energy Chemistry 2022年第1期31卷 116-128,I0004页

作者： Vittorio Marangon Daniele Di Lecce Dan J.L.Brett Paul R.Shearing Jusef Hassoun University of Ferrara Department of Chemical and Pharmaceutical SciencesVia Fossato di Mortara 17Ferrara44121Italy Electrochemical Innovation Lab Department of Chemical EngineeringUCLLondon WC1E 7JEUnited Kingdom The Faraday Institution Quad OneBecquerel AveHarwell CampusDidcot OX11 ORAUnited Kingdom National Interuniversity Consortium of Materials Science and Technology(INSTM) University of Ferrara Research UnitUniversity of FerraraVia Fossato di Mortara17Ferrara 44121Italy

Bulk sulfur incorporating 3 wt% gold nano-powder is investigated as possible candidate to maximize the fraction of active material in the Li-S battery cathode.The material is prepared via simple mixing of gold with molten sulfur at 120℃,quenching at room temperature,and grinding.Our comprehensive study reports relevant electrochemical data,advanced X-ray computed tomography(CT)imaging of the positive and negative electrodes,and a thorough structural and morphological characterization of the S:Au 97:3 w/w composite.This cathode exhibits high rate capability within the range from C/10 to 1C,a maximum capacity above 1300 mAh gs^(-1),and capacity retention between 85%and 91%after 100 cycles at 1C and C/3 rates.The novel formulation enables a sulfur fraction in the composite cathode film as high as 78 wt%,an active material loading of 5.7 mg cm^(-2),and an electrolyte/sulfur(E/S)ratio of 5μL mg^(-1),which lead to a maximum areal capacity of 5.4 mAh cm^(-2).X-ray CT at the micro-and nanoscale reveals the microstructural features of the positive electrode that favor fast conversion kinetics in the battery.Quantitative analysis of sulfur distribution in the porous cathode displays that electrodeposition during the initial cycle may trigger an activation process in the cell leading to improved performance.Furthermore,the tomography study reveals the characteristics of the lithium anode and the cell separator upon a galvanostatic test prolonged over 300 cycles at a 2C rate.

关键词： lithium-sulfur battery sulfur loading Electrolyte/sulfur ratio Gold nanoparticles X-ray tomography

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High-yield red phosphorus sponge mediated robust lithium-sulfur battery

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Nano Research 2023年第6期16卷 8329-8337页

作者： Zheng Luo Shusheng Tao Ye Tian Hanyu Tu Laiqiang Xu Wentao Deng Guoqiang Zou Hongshuai Hou Xiaobo Ji State Key Laboratory of Powder Metallurgy College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083China

Although lithium-sulfur(Li-S)batteries with high specific energy exhibit great potential for next-generation energy-storage systems,their practical applications are limited by the growth of Li dendrites and lithium polysulfides(LiPSs)shuttling.Herein,a highly porous red phosphorus sponge(HPPS)with well distributed pore structure was efficiently prepared via a facile and largescale hydrothermal process for polysulfides adsorption and dendrite suppression.As experimental demonstrated,the porous red phosphorus modified separator with increased active site greatly promotes the chemisorption of LiPSs to efficiently immobilize the active sulfur within the cathode section,while Li metal anode activated by Li_(3)P interlayer with abundant ionically conductive channels significantly eliminates the barrier for uniform Li^(+)permeation across the interlayer,contributing to the enhanced stability for both S cathode and Li anode.Mediated by the HPPS,long-term stability of 1,200 h with minor voltage hysteresis is achieved in symmetric cells with Li_(3)P@Li electrode while Li-S half-cell based on HPPS modified separator delivers an outperformed reversibility of 783.0 mAh·g^(−1)after 300 cycles as well as high-rate performance of 694.5 mAh·g^(−1)at 3 C,which further boosts the HPPS tuned full cells in practical S loading(3 mg·cm^(−2))and thin Li3P@Li electrode(100μm)with a capacity retention of 71.8%after 200 cycles at 0.5 C.This work provides a cost-effective and metal free mediator for simultaneously alleviating the fundamental issues of both S cathode and Li anode towards high energy density and long cycle life Li-S full batteries.

关键词： lithium-sulfur battery red phosphorus sponge separator chemical adsorption Li dendrite

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Nitrogen-rich azoles as trifunctional electrolyte additives for high-performance lithium-sulfur battery

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Journal of Energy Chemistry 2022年第8期31卷 572-579,I0015页

作者： Dan-Yang Wang Wenmin Wang Fengli Li Xin Li Wei Guo Yongzhu Fu College of Chemistry Zhengzhou UniversityZhengzhou 450001HenanChina Hefei National Laboratory for Physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026AnhuiChina College of Chemistry Chemical Engineering and Materials ScienceZaozhuang UniversityZaozhuang 277160ShandongChina

Rechargeable lithium-sulfur(Li-S)batteries are considered one of the most promising energy storage techniques owing to the high theoretical energy density.However,challenges still remain such as the shuttle effect of lithium polysulfides(LPSs)and the instability of lithium metal anode.Herein,we propose to use nitrogen-rich azoles,i.e.,triazole(Ta)and tetrazole(Tta),as trifunctional electrolyte additives for Li-S batteries.The azoles afford strong lithiophilicity for the chemisorption of LPSs.The density functional theory and experimental analysis verify the presence of Li bonds between the azoles and LPSs.The azoles can also interact with lithium salt in the electrolyte,leading to increase ionic conductivity and lithiumion transference number.Moreover,the azoles render particle-like lithium deposition on the lithium metal anode,leading to superlong cycling of a Li symmetric cell.The Li-S batteries with Ta and Tta exhibit the initial discharge capacity of 1425.5 and 1322.2 m Ah g^(-1),respectively,at 0.2 C rate,and promising cycling stability.They also enable enhanced cycling performance of a Li-organosulfide battery.

关键词： Azole Electrolyte additive lithium-sulfur battery Chemisorption Organosulfide

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Hierarchically porous nitrogen-doped carbon foams decorated with zinc nanodots as high-performance sulfur hosts for lithium-sulfur battery

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Chinese Chemical Letters 2021年第9期32卷 2919-2922页

作者： Zhibo Liu Li Wang Wantai Yang State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China School of Materials Science and Engineering Beijing University of Chemical TechnologyBeijing 100029China Beijing Advanced Innovation Centre for Soft Matter Science and Engineering Beijing University of Chemical TechnologyBeijing 100029China

To prevent polysulfides from dissolution into electrolyte,we propose a novel and simple approach to nitrogen-doped carbon foams which contain hierarchically porous structure and are decorated with zinc nanodots through one-pot carbonization and activation process.These carbon foams,which serve as hosts for sulfur in lithium battery,can provide a conducting network and shorter diffusion length for Liions.Specially,the zinc nanodots derived from the carbothermal reaction of ZnCl_(2) at high temperature can interact with sulfur/polysulfides by strong chemisorption.In addition,the zinc nanodots can also facilitate the conversion reaction between Li_(2)S_(x)(2sulfur utility and large capacity.

关键词： Nitrogen-doped carbon foams Hierarchically porous lithium-sulfur battery

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A systematic correlation between morphology of porous carbon cathode and electrolyte in lithium-sulfur battery

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Journal of Energy Chemistry 2021年第10期30卷 561-573,I0014页

作者： Jihyeon Park Seoyoung Yoon Seoyeah Oh Jiyoon Kim Dongjun Kim Geonho Kim Jiyeon Lee Myeong Jun Song Ilto Kim Kwonnam Sohn Jiwon Kim School of Integrated Technology College of EngineeringYonsei University85 Songdogwahak-roYeonsu-guIncheon 21983Republic of Korea Integrated Science and Engineering Division Underwood International CollegeYonsei University85 Songdogwahak-roYeonsu-guIncheon 21983Republic of Korea Integrated Biotechnology and Translational Medicine Graduate SchoolYonsei University85 Songdogwahak-roYeonsu-guIncheon 21983Republic of Korea LG Chem. LG Science Park30 Magokjungang 10-roGangseo-guSeoul 07796Republic of Korea

Porous carbon has been applied for lithium-sulfur battery cathodes,and carbonized metal-organic framework(MOF)is advantageous in tuning the morphology.Herein,we have systematically synthesized water-distorted MOF(WDM)derived porous carbon via controlling the proportion of both water in a mixed solvent(dimethylformamide and water)and ligand in MOF-5 precursors(metal and ligand),which is categorized by its morphology(i.e.Cracked stone(closed),Tassel(open)and Intermediate(semi-open)).For example,decrease in water and increase in ligand content induce Cracked stone WDMs which showed the highest specific surface area(2742-2990 m^(2)/g)and pore volume(2.81-3.28 cm^(3)/g)after carbonization.Morphological effect of carbonized WDMs(CWDMs)on battery performance was examined by introducing electrolytes with different sulfur reduction mechanisms(i.e.DOL/DME and ACN_(2) LiTFSITTE):Closed framework effectively confines polysulfide,whereas open framework enhances electrolyte accessibility.The initial capacities of the batteries were in the following order:Cracked stone>Intermediate>Tassel for DOL/DME and Intermediate>Tassel>Cracked stone for ACN_(2) LiTFSI-TTE.To note,Intermediate CWDM exhibited the highest initial capacity and retained capacity after 100 cycles(1398 and 747 mAh/g)in ACN_(2) LiTFSI-TTE electrolyte having advantages from both open and closed frameworks.In sum,we could correlate cathode morphology(openness and pore structure)and electrolyte type(i.***.polysulfide solubility)with lithium-sulfur battery performance.

关键词： lithium-sulfur battery Metal-organic framework Hierarchical porous carbon cathode Morphology control Electrolyte lithium polysulfide solubility

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In-situ assembly of TiO2 with high exposure of(001)facets on three-dimensional porous graphene aerogel for lithium-sulfur battery

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Journal of Energy Chemistry 2020年第10期29卷 316-322页

作者： Ming Wang Shunyuan Tan Shuting Kan Yufeng Wu Shangbin Sang Kaiyu Liu Hongtao Liu Hunan Provincial Key Laboratory of Chemical Power Sources Hunan Provincial Key Laboratory of Efficient and Clean Utilization of Manganese ResourcesCollege of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083HunanChina

Resulting from the development of electric vehicles,high energy-density Li-S batteries have recently attracted ever-increasing attentions worldwide.However,continuous dissolution of cathodic sulfur and followed shuttle effect of polysulfides lead to very limited service lifetime for currently-applied Li-S batteries.Herein,a 3 D porous graphene aerogel(GA)decorated with high exposure of anatase TiO2(001)nanoplatelets is proposed as robust host to immobilize cathodic sulfur.Compared with commonly used TiO2(101)nanoparticles,the Ti O2(001)nanoplatelets have highly matched lattices with graphene(002)nanosheets,thus facilitating the electronic transfer.The in-site assembled TiO2@GA host exhibits superior sulfur-immobilized capability,which cannot only entrap sulfur by physical confinement,but also capture dissoluble sulfurous species by chemical bonding.The fabricated S@TiO2@GA cathode shows excellent electrochemical performance with high discharge capacity,superior rate capability,and durable cycling stability as well,supposed to be a promising cathode for high-performance Li-S battery applications.

关键词： lithium-sulfur battery Porous graphene aerogel Anatase(001) Immobilization of sulfur Electrochemical performance

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Promoting performance of lithium-sulfur battery via in situ sulfur reduced graphite oxide coating

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Rare Metals 2021年第2期40卷 417-424页

作者： Yuan Li Xiao-Tian Guo Song-Tao Zhang Huan Pang Department of Pharmacy Jiangsu Food and Pharmaceutical Science CollegeHuai’an223003China School of Chemistry and Chemical Engineering Guangling CollegeYangzhou UniversityYangzhou225000China

Activated graphene/sulfur structure sheathed in a flexible graphene layer is presented as the cathode material of lithium-sulfur battery.The surface coating graphite oxide sheets are reduced by a one-step in situ sulfur reduction method under vacuum at 600℃without any additional reductant.The high reduction degree of in situ sulfur reduced graphite oxide(RGO)coating layer will facilitate the rapid charge transfer at high current rate.The flexible encapsulated RGO structure will retard the diffusion of polysulfides and adjust the volume change of sulfur in cycling.As a result,the electrochemical evaluation of the RGO-activated graphene(AG)/S electrode demonstrates superior capacity,cycling and rate performance.The RGO-AG/S electrode with 60 wt%sulfur loading achieves a stable cyclability over 2000 galvanostatic charge/discharge process(capacity-fade rate of only 0.03%per cycle at1600 mA·g^(-1)).The average Coulombic efficiency remains at~96%with no electrolyte additives(such as LiNO_(3)).The outstanding property of RGO-AG/S electrode is attributed to the distinctive in situ sulfur RGOcoated hierarchical texture.

关键词： lithium-sulfur battery Surface coating In situ Activated graphene Long-term stability

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利用钴酸锂构筑高体积比容量和高质量比容量硫电极

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Science China Materials 2021年第6期64卷 1343-1354页

作者：刘亚涛王璐刘胜李国然高学平 Institute of New Energy Material Chemistry School of Materials Science and EngineeringNankai UniversityTianjin 300350China

锂-硫电池的质量能量密度较高,但其体积能量密度却并不理想.为了提高锂-硫电池的体积能量密度,需要重点改善复合硫电极的结构和密度.本研究引入高密度的钴酸锂纳米纤维作为硫的载体材料.钴酸锂的振实密度高达2.26 g cm^(−3),硫/钴酸锂... 详细信息

锂-硫电池的质量能量密度较高,但其体积能量密度却并不理想.为了提高锂-硫电池的体积能量密度,需要重点改善复合硫电极的结构和密度.本研究引入高密度的钴酸锂纳米纤维作为硫的载体材料.钴酸锂的振实密度高达2.26 g cm^(−3),硫/钴酸锂电极的密度和孔隙率分别为0.85 g cm^(−3)和61.2%.研究发现,钴酸锂是一种优异的电催化剂,可以加速活性物质硫的反应速率.因此,硫/钴酸锂正极兼具致密的电极结构和良好的电化学活性,其体积能量密度得到显著提升,并同时保持较高的质量能量密度.当硫的面负载量为5.1 mg cm^(−2)时,整体硫/钴酸锂电极的体积和质量比容量分别为724 mA h cm^(−3)和848 mA h g^(−1).此外,钴酸锂可以减缓多硫化锂的穿梭并降低多硫化锂对锂负极的腐蚀,提高锂负极的稳定性.

关键词： lithium-sulfur battery sulfur cathode volumetric energy density lithium cobalt oxide catalytic activity

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Vapor deposition of aluminium oxide into N-rich mesoporous carbon framework as a reversible sulfur host for lithium-sulfur battery cathode

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Nano Research 2021年第1期14卷 131-138页

作者： Fei Sun Zhibin Qu Hua Wang Xiaoyan Liu Tong Pei Rui Han Jihui Gao Guangbo Zhao Yunfeng Lu School of Energy Science and Engineering Harbin Institute of TechnologyHarbin 150001China Department of Chemistry Shanghai Normal UniversityShanghai 150001China Department of Chemical and Biomolecular Engineering University of CaliforniaLos AngelesCA 90095USA

Restraining the shuttle effects of lithium polysulfides is the key to improve the cycling reversibility and stability of lithium-sulfur(Li-S)batteries for which design of robust sulfur hosts has been regarded as the most effective strategy.In this work,we report a new type of hybrid sulfur host which is composed of Al_(2)O_(3) homogenously decorated in nitrogen-rich mesoporous carbon framework(NMC-Al_(2)O_(3)).The NMC-Al_(2)O_(3) hybrid host features a poly-dispersed spherical morphology and a mesoporous configuration with high surface area and large pore volume that can accommodate a high sulfur content up to 73.5 wt.%.As a result,the fabricated NMC-Al_(2)O_(3)-S cathode exhibits all-round improvements in electrochemical properties in term of capacities(1,212 mAh·g^(-1)at 0.2 C;755 mAh·g^(-1)at 2 C),cycling charge-discharge reversibility(sustainably 100%efficiencies)and stability(1,000 cycles with only 0.023%capacity decay per cycle at 0.5 C).By contrast,the Al_(2)O_(3)-free NMC-S cathode shows both decreased capacities and rapidly descending Coulombic efficiencies during cycling.Density functional theory(DFH")calculations further reveal that the implanted Al_(2)O_(3) can greatly enhance the chemical adsorption and catalytic conversion for various lithium polysulfides and thereby effectively prevent the polysulfide shuttling and significantly improve the utilizability,reversibility and stability of sulfur cathode.

关键词： lithium-sulfur battery aluminium oxide sulfur host nitrogen-rich carbon mesoporous structure

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