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Suitable Lithium polysulfides diffusion and adsorption on CNTs@TiO_(2)-bronze nanosheets surface for high-performance lithium-sulfur batteries

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Nano Research 2022年第2期15卷 933-941页

作者： Mengmeng Zhen Keliang Jiang Sheng-Qi Guo Boxiong Shen Huiling Liu Tianjin Key Laboratory of Clean Energy and Pollution Control School of Energy and Environmental EngineeringHebei University oj TechnologyTianjin 300401China Tianjin Key Laboratory of Advanced Functional Porous Materials and Center for Electron Microscopy Institute for New Energy Materials&Low-Carbon TechnologiesSchool of Materials Science and EngineeringTianjin University of TechnologyTianjin 300071China

The shuttle effect of Lithium polysulfides(UPSs)in lithium-sulfur batteries(LSBs)has been hampered their commercialization.Metal oxides as separator modifications can suppress the shuttle effect.Since there is no direct electron transport between metal oxides and UPSs,absorbed UPSs should be diffused from the surface of metal oxides to the carbon matrix to go through redox reactions.If diffusivity of UPSs from metal oxides surface to carbon substrate is poor,it would hinder the redox reactions of LiPSs.Nevertheless,researchers tend to focus on the adsorption and overlook the diffusion of UPSs.Herein,same morphology and different crystal phase of TiO_(2) nanosheets grown on carbon nanotubes(CNTs@TiO_(2)-bronze and CNTs@TiO_(2)-anatase)have been designed via a simple approach.Compared with CNTs and CNTs@TiO_(2)-anatase composites,the battery with CNTs@TiO_(2)-bronze modified separator delivers higher specific capacities and stronger cycling stability,especially at high current rates(~472 mAh·g^(-1) at 2.0 C after 1,000 cycles).Adsorption tests,density functional theory calculations and electrochemical performance evaluations indicate that suitable diffusion and adsorption for LiPSs on the CNTs@TiO_(2)-B surface can effectively capture LiPSs and promote the redox reaction,leading to the superior cycling performances.

关键词： Lithium polysulfides Li ion diffusion adsorption TiO_(2)-bronze surface long-term cycling performances

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Inhibiting shuttle effect of Lithium polysulfides by double metal selenides for high-performance lithium-sulfur batteries

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Rare Metals 2024年第6期43卷 2546-2559页

作者： Lei Li Xue-Jing Yang Yi-Yang Li Bo Jin Hui Liu Meng-Yang Cui Dong-Bo Guan Xing-You Lang Qing Jiang Jilin University and College of Materials Science and Engineering Key Laboratory of Automobile Materials Ministry of Education

lithium-sulfur batteries(LSBs) have attracted the attention of more and more researchers due to the advantages of high energy density,environmental friendliness,and low production cost.However,the low electronic conductivity of active material and shuttling effect of Lithium polysulfides(LiPSs) limit the commercial development of LSBs.To solve these problems,we design a core-shell composite with nitrogen-doped carbon(NC) and two types of selenides(FeSe2-NC@ZnSe-NC).The FeSe2-NC@ZnSe-NC has a strong adsorption capacity,and can effectively adsorb LiPSs.At the same time,it also effectively alleviates the shuttling effect of LiPSs,and improves the utilization of the active substance during the charge/discharge reaction processes.The mechanism involved in FeSe2-NC@ZnSe-NC is demonstrated by both experiments and density-functional theory(DFT) calculations.The electrochemical test results indicate that LSB with S/FeSe2-NC@ZnSe-NC delivers an initial discharge capacity of 1260 mAh·g-1at 0.2C.And after 500 cycles at 1C,the capacity decay rate per cycle is 0.031%,and the capacity retention rate is 85%.The FeSe2-NC@ZnSe-NC core-shell structure verifies a rational strategy to construct an electrode material for high-performance LSBs.

关键词： lithium–sulfur batteries Shuttling effect Metal selenide Nitrogen-doped carbon Lithium polysulfides

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Tuning the solubility of polysulfides for constructing practical lithium-sulfur battery

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Journal of Energy Chemistry 2024年第8期95卷 611-617页

作者： Jiapeng Li Jianlong Cong Haijin Ji Ting Shi Lixia Yuan Yunhui Huang State Key Laboratory of Material Processing and Die & Mold Technology Huazhong University of Science and Technology School of Materials Science and Engineering

Li-S batteries are regarded as one of the most promising candidates for next-generation battery systems with high energy density and low cost.However,the dissolution-precipitation reaction mechanism of the sulfur(S) cathode enhances the kinetics of the redox processes of the insulating sulfu r,which also arouses the notorious shuttle effect,leading to serious loss of S species and corrosion of Li anode.To get a balance between the shuttle restraining and the kinetic property,a combined strategy of electrolyte regulation and cathode modification is proposed via introducing 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoroprpyl ether(HFE) instead of 1,2-dimethoxyethane(DME),and SeS7instead of S8.The introduction of HFE tunes the solvation structure of the LiTFSI and the dissolution of intermediate polysulfides with Se doping(LiPSSes),and optimize the interface stability of the Li anode simultaneously.The minor Se substitution compensates the decrease in kinetic due to the decreased solubility of LiPSs.In this way,the Li-SeS7batteries deliver a reversible capacity of 1062 and 1037 mAh g-1with 2.0 and 5.5 mg SeS7cm-2loading condition,respectively.Besides,an electrolyte-electrode loading model is established to explain the relationship between the optimal electrolyte and cathode loading.It makes more sense to guide the electrolyte design for practical Li-S batteries.

关键词： Interface Li-S batteries Lithium polysulfides Se doping Shuttle effect Solubility

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Engineering Strategies for Suppressing the Shuttle Effect in lithium–Sulfur Batteries

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Nano-Micro Letters 2024年第1期16卷 187-221页

作者： Jiayi Li Li Gao Fengying Pan Cheng Gong Limeng Sun Hong Gao Jinqiang Zhang Yufei Zhao Guoxiu Wang Hao Liu Joint International Laboratory On Environmental and Energy Frontier Materials School of Environmental and Chemical EngineeringShanghai UniversityShanghaiPeople’s Republic of China Centre for Clean Energy Technology University of Technology SydneyBroadwaySydneyNSW 2007Australia

lithium–sulfur(Li–S)batteries are supposed to be one of the most potential next-generation batteries owing to their high theoretical capacity and low cost.Nevertheless,the shuttle effect of firm multi-step two-electron reaction between sulfur and lithium in liquid electrolyte makes the capacity much smaller than the theoretical value.Many methods were proposed for inhibiting the shuttle effect of polysulfide,improving corresponding redox kinetics and enhancing the integral performance of Li–S batteries.Here,we will comprehensively and systematically summarize the strategies for inhibiting the shuttle effect from all components of Li–S batteries.First,the electrochemical principles/mechanism and origin of the shuttle effect are described in detail.Moreover,the efficient strategies,including boosting the sulfur conversion rate of sulfur,confining sulfur or Lithium polysulfides(LPS)within cathode host,confining LPS in the shield layer,and preventing LPS from contacting the anode,will be discussed to suppress the shuttle effect.Then,recent advances in inhibition of shuttle effect in cathode,electrolyte,separator,and anode with the aforementioned strategies have been summarized to direct the further design of efficient materials for Li–S batteries.Finally,we present prospects for inhibition of the LPS shuttle and potential development directions in Li–S batteries.

关键词： Shuttle effect Designed strategies Li-S battery Lithium polysulfides

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Isolated diatomic Zn-Co metal–nitrogen/oxygen sites with synergistic effect on fast catalytic kinetics of sulfur species in Li-S battery

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Journal of Energy Chemistry 2023年第4期79卷 505-514页

作者： Chun-Lei Song Qiao-Tong He Zhongyi Zeng Jing-Yan Chen Tian Wen Yu-Xiao Huang Liu-Chun Zhuang Wei Yi Yue-Peng Cai Xu-Jia Hong School of Chemistry South China Normal UniversityGuangzhou 510006GuangdongChina Guangzhou Municipal and Guangdong Provincial Key Laboratory of Molecular Target&Clinical Pharmacology the NMPA and State Key Laboratory of Respiratory DiseaseSchool of Pharmaceutical Sciences&the Fifth Affiliated Hospital Guangzhou Medical UniversityGuangzhou 511436GuangdongChina

lithium-sulfur batteries are severely restricted by low electronic conductivity of sulfur and Li_(2)S,shuttle effect,and slow conversion reaction of Lithium polysulfides(LiPSs).Herein,we report a facile and highyield strategy for synthesizing dual-core single-atom catalyst(ZnCoN_(4)O_(2)/CN)with atomically dispersed nitrogen/oxygen-coordinated Zn-Co sites on carbon nanosheets.Based on density functional theory(DFT)calculations and LiPSs conversion catalytic ability,ZnCoN_(4)O_(2)/CN provides dual-atom sites of Zn and Co,which could facilitate Li^(+)transport and Li_(2)S diffusion,and catalyze LiPSs conversion more effectively than homonuclear bimetallic single-atom catalysts or their simple mixture and previously reported singleatom catalysts.Li-S cell with ZnCoN_(4)O_(2)/CN modified separator showed excellent rate performance(789.4 mA h g^(-1)at 5 C)and stable long cycle performance(0.05%capacity decay rate at 6C with 1000cycles,outperforming currently reported single atomic catalysts for LiPSs conversion.This work highlights the important role of metal active centers and provides a strategy for producing multifunctional dual-core single atom catalysts for high-performance Li-S cells.

关键词： Dual-core single-atom catalysts Lithium polysulfides Fast catalytic kinetics Li_(2)S diffusion Li-S battery

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Enhanced polysulfide redox kinetics by niobium oxynitrides via insitu adsorptive and catalytic effect in wide temperature range

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Nano Research 2022年第7期15卷 6200-6207页

作者： Benben Wei Chaoqun Shang Qiao Cu Le Hu Xuelian Fu Guofu Zhou Xin Wang School of Materials Science and Engineering&Hubei Key Laboratory of Plasma Chemistry and Advanced Materials Wuhan Institute of TechnologyWuhan 430205China Faculty of Materials Science and Chemistry China University of GeosciencesWuhan 430074China Guangdong Provincial Key Laboratory of Optical Information Materials and Technology&South China Academy of Advanced Optoelectronics South China Normal UniversityGuangzhou 510006China School of Materials Science and Engineering&State Key Laboratory of Material Processing and Die and Mold Technology Huazhong University of Science and TechnologyWuhan 430074China

The development of Li-S batteries(LSBs)is hindered by the low utilization of S species and sluggish redox reaction kinetics.Polar metal oxides always possess high adsorption to polar S species,while conductive metal nitrides show fast electron transport and ensure fast redox reaction of S species.The combination merits of metal oxides and metal nitrides in one provide an effective strategy to improve the electrochemical performance of LSBs.In this work,defect design of niobium oxynitrides highly dispersed on graphene(NbON-G)is evaluated as effective trapper and catalyst for S species.Owning to the effective structural merits including enriched active sites,alleviated volume variation,defect modulated electronic property,and in-situ chemisorption and catalytic conversion of soluble Lithium polysulfides(LiPSs),the LSBs with NbON-G modified separator show remarkably enhanced performance compared to NbN-G and Nb_(2)O_(5)-G.Surprisingly,even at low temperature of−40°C,the LSBs with NbON-G can operate for 1,000 cycles with 0.04%capacity decay per cycle(Rate:2 C).

关键词： Lithium polysulfides Li-S batteries niobium oxynitrides catalyst low temperature

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Premature deposition of lithium polysulfide in lithium-sulfur batteries

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Journal of Energy Chemistry 2023年第7期82卷 507-512,I0011页

作者： Zi-Xian Chen Yu-Tong Zhang Chen-Xi Bi Meng Zhao Rui Zhang Bo-Quan Li Jia-Qi Huang School of Materials Science and Engineering Beijing Institute of TechnologyBeijing 100081China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China

lithium-sulfur(Li-S)batteries have attracted extensive attention due to ultrahigh theoretical energy density of 2600 Wh kg^(-1).Liquid-solid deposition from dissolved Lithium polysulfides(LiPSs)to solid lithium sulfide(Li_(2)S)largely determines the actual battery performances.Herein,a premature liquidsolid deposition process of LiPSs is revealed at higher thermodynamic potential than Li_(2)S deposition in Li-S batteries.The premature solid deposit exhibits higher chemical state and hemispherical morphology in comparison with Li_(2)S,and the premature deposition process is slower in kinetics and higher in deposition dimension.Accordingly,a supersaturation deposition mechanism is proposed to rationalize the above findings based on thermodynamic simulation.This work demonstrates a unique premature liquid-solid deposition process of Li-S batteries.

关键词： lithium-sulfur batteries Lithium polysulfides Liquid-solid deposition Supersaturation

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Boosting sulfur redox kinetics by a pentacenetetrone redox mediator for high-energy-density lithium-sulfur batteries

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Nano Research 2023年第6期16卷 8253-8259页

作者： Yan-Qi Peng Meng Zhao Zi-Xian Chen Qian Cheng Yiran Liu Xi-Yao Li Yun-Wei Song Bo-Quan Li Jia-Qi Huang School of Materials Science and Engineering Beijing Institute of TechnologyBeijing 100081China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

lithium-sulfur(Li-S)battery is considered as a promising energy storage system due to its ultrahigh theoretical energy density of 2,600 Wh·kg^(−1).Redox mediation strategies have been proposed to promote the sluggish sulfur redox kinetics.Nevertheless,the applicability of redox mediators in practical high-energy-density Li-S batteries has seldomly been manifested.In this work,5,7,12,14-pentacenetetrone(PT)is proposed as an effective redox mediator to promote the sulfur redox kinetics under practical working conditions.A high initial specific discharge capacity of 993 mAh·g^(−1) is achieved at 0.1 C with high-sulfur-loading cathodes of 4.0 mgS·cm^(−2)and low electrolyte/sulfur(E/S)ratio of 5μL·mg_(S)^(−1).More importantly,practical Li-S pouch cells with the PT mediator realize an actual initial energy density of 344 Wh·kg^(−1)and cycle stably for 20 cycles wih a high capacity retention of 88%.This work proposes an effective redox mediator and further verifies the redox mediation strategy for practical high-energydensity Li-S batteries.

关键词： lithium-sulfur batteries Lithium polysulfides redox mediation sulfur redox kinetics pouch cells

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Constructing a 700 Wh kg^(-1)-level rechargeable lithium-sulfur pouch cell

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Journal of Energy Chemistry 2023年第1期76卷 181-186,I0005页

作者： Qian Cheng Zi-Xian Chen Xi-Yao Li Li-Peng Hou Chen-Xi Bi Xue-Qiang Zhang Jia-Qi Huang Bo-Quan Li School of Materials Science and Engineering Beijing Institute of TechnologyBeijing 100081China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

lithium–sulfur(Li–S)batteries are considered as highly promising energy storage devices because of their ultrahigh theoretical energy density of 2600 Wh kg^(-1).The highest practical energy density of Li–S batteries reported at pouch cell level has exceeded 500 Wh kg^(-1),which significantly surpasses that of lithium-ion batteries.Herein,a 700 Wh kg^(-1)-level Li–S pouch cell is successfully constructed.The pouch cell is designed at 6 Ah level with high-sulfur-loading cathodes of 7.4 mgScm^(-2),limited anode excess(50μm in thickness),and lean electrolyte(electrolyte to sulfur ratio of 1.7 gelectrolyteg^(-1)S).Accordingly,an ultrahigh specific capacity of 1563 m A h g^(-1)is achieved with the addition of a redox comediator to afford a practical energy density of 695 Wh kg^(-1)based on the total mass of all components.The pouch cell can operate stably for three cycles and then failed due to rapidly increased polarization at the second discharge plateau.According to failure analysis,electrolyte exhaustion is suggested as the key limiting factor.This work achieves a significant breakthrough in constructing high-energy-density Li–S batteries and propels the development of Li–S batteries toward practical working conditions.

关键词： lithium–sulfur batteries Pouch cell High energy density Lithium polysulfides

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Ion shielding functional separator using halloysite containing a negative functional moiety for stability improvement of Li–S batteries

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Journal of Energy Chemistry 2021年第9期30卷 334-340页

作者： Yong Min Kwon Jihoon Kim Kuk Young Cho Sukeun Yoon Division of Advanced Materials Engineering&Institute for Rare Metals Kongju National UniversityChungnam 31080Republic of Korea Department of Materials Science and Chemical Engineering Hanyang UniversityGyeonggi 15588Republic of Korea

lithium–sulfur batteries are one of the attractive next-generation energy storage systems owing to theienvironmental friendliness,low cost,and high specific energy densities.However,the low electrical conductivity of sulfur,shuttling of soluble intermediate polysulfides between electrodes,and low capacitretention have hampered their commercial use.To address these issues,we use a halloysitemodulated(H-M)separator in a lithium–sulfur battery to mitigate the shuttling problem.The H-M separator acts as a mutual Coulombic repulsion in lithium-sulfur batteries,thereby selectively permitting Lions and efficiently suppressing the transfer of undesired Lithium polysulfides to the Li anode sideMoreover,the use of halloysite switches the surface of the separator from hydrophobic to hydrophilicconsequently improving the electrolyte wettability and adhesion between the separator and cathodeWhen sulfur-multi-walled carbon nanotube(S-MWCNT)composites are used as cathode active materialsa lithium–sulfur battery with an H-M separator exhibits first discharge and charge capacities of 1587 an1527 m Ah g-1,respectively.Moreover,there is a consistent capacity retention up to 100 cyclesAccordingly,our approach demonstrates an economical and easily accessible strategy for commercialization of lithium–sulfur batteries.

关键词： Li–S batteries Halloysite Ion shielding Negative functional moiety Lithium polysulfides

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