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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 Key Laboratory of Automobile Materials Ministry of Educationand College of Materials Science and EngineeringJilin University

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

Insight into lithium–sulfur batteries performance enhancement: from metal nanoparticles to metal nanoclusters to single metal atoms

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Tungsten 2024年第3期6卷 504-521页

作者： Shuang Ma Qing-Ling Ruan Xue-Cheng Liu Gui-Jun Zhu Die Yuan Ling-Qiao Hu Yu-Mei Huang Xing-Xing Gu Chongqing Key Laboratory of Catalysis and New Environmental Materials College of Environment and Resources Chongqing Technology and Business University National Research Base of Intelligent Manufacturing Service Chongqing Technology and Business University

lithium-sulfur(Li-S) batteries have attracted much attention and developed rapidly in recent years due to their high energy density,low cost,and environment-friendly.However,its commercialization process still encounters various obstacles.Among them,the sulfur cathode is easy to dissolve and shuttle,resulting in the loss of active substances and the severe growth of lithium anode dendrites,which is one of the biggest obstacles.Improving the redox conversion kinetics of sulfur cathode is expected to fundamentally alleviate the shuttle phenomenon of poly sulfides.Therefore,this paper reviews the effects of metal nanoparticles to metal nanoclusters to metal single-atom catalysts on improving the redox of Li-S batteries,to let researchers better understand the size effect on the kinetics of sulfur cathodes in Li-S batteries,which will provide important guidance for the future large-scale commercialization of Li-S batteries.

关键词： lithium–sulfur batteries Metal nanoparticles Metal nanoclusters Metal single atoms Size effects

Metal phosphides and borides as the catalytic host of sulfur cathode for lithium–sulfur batteries

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International Journal of Minerals,Metallurgy and Materials 2022年第5期29卷 990-1002页

作者： Rui Gao Zhenyu Wang Sheng Liu Guangjie Shao Xueping Gao College of Environmental and Chemical Engineering Yanshan UniversityQinhuangdao 066004China School of Materials Science and Engineering Nankai UniversityTianjin 300350China

lithium−sulfur batteries are one of the most competitive high-energy batteries due to their high theoretical energy density of _(2)600 W·h·kg^(−1).However,their commercialization is limited by poor cycle stability mainly due to the low intrinsic electrical conductivity of sulfur and its discharged products(Li_(2)S_(2)/Li_(2)S),the sluggish reaction kinetics of sulfur cathode,and the“shuttle effect”of soluble intermediate lithi-um polysulfides in ether-based electrolyte.To address these challenges,catalytic hosts have recently been introduced in sulfur cathodes to en-hance the conversion of soluble polysulfides to the final solid products and thus prevent the dissolution and loss of active-sulfur material.In this review,we summarize the recent progress on the use of metal phosphides and borides of different dimensions as the catalytic host of sulfur cathodes and demonstrate the catalytic conversion mechanism of sulfur cathodes with the help of metal phosphides and borides for high-en-ergy and long-life lithium-sulfur batteries.Finally,future outlooks are proposed on developing advanced catalytic host materials to improve battery performance.

关键词： lithium–sulfur batteries sulfur cathode catalytic host metal phosphides metal borides

An integrated approach to improve the performance of lean–electrolyte lithium–sulfur batteries

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Journal of Energy Chemistry 2022年第4期31卷 585-592页

作者： Hualin Ye Jianguo Sun Yun Zhao Jim Yang Lee Department of Chemical and Biomolecular Engineering National University of Singapore119260Singapore Department of Mechanical Engineering National University of Singapore117575Singapore

While the sulfur conversion reaction kinetics in Li–S batteries is nowadays improved by the use of appropriate electrocatalysts,it remains a challenge for the batteries to perform well under the lean electrolyte condition where polysulfide shuttle,electrode passivation and the loss of electrolyte due to side reactions,are aggravated.These challenges are addressed in this study by the tandem use of a polysulfide conversion catalyst and a redox–targeting mediator in a gel sulfur cathode.Specifically,the gel cathode reduces the polysulfide mobility and hence the polysulfide shuttle and the passivation of the lithium anode by the crossover polysulfides.The redox mediator restrains the deposition of inactive sulfur species in the cathode thereby enabling the Fe–N and Co–N co–doped carbon catalyst to prolong its catalytic activity.Consequently,the integrated catalytic system is able to increase the discharge capacity of high–loading (6.8 mg cm^(-2)) lean–electrolyte (4.0μL mg^(-1)) Li–S batteries from~630 to~1316 m Ah g^(-1),concurrently with an improvement of the cycle life (600 cycles with 46%capacity retention at 1.0 m A cm^(-2)).Redox mediator assisted catalysis in a gel cathode is therefore an effective strategy to extend the application of the sulfur conversion catalyst in lean electrolyte Li–S batteries.

关键词： Redox mediators Gel electrolytes Polysulfide catalysis Lean electrolyte lithium–sulfur batteries

Uncovering the solid-phase conversion mechanism via a new range of organosulfur polymer composite cathodes for lithium-sulfur batteries

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能源化学:英文版 2023年第9期84卷 459-466页

作者： Xiang Li Dezhong Liu Ziyi Cao Yaqi Liao Zexiao Cheng Jie Chen Kai Yuan Xing Lin Zhen Li Yunhui Huang Lixia Yuan State Key Laboratory of Material Processing and Die&Mold Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiChina

The sulfur cathodes operating via solid phase conversion of sulfur have natural advantages in suppressing polysulfide dissolution and lowering the electrolyte dosage,and thus realizing significant improvements in both cycle life and energy density.To realize an ideal solid-phase conversion of sulfur,a deep understanding of the regulation path of reaction mechanism and a corresponding intentional material and/or cathode design are highly essential.Herein,via covalently fixing of sulfur onto the triallyl isocyanurate,a series of S-triallyl isocyanurate organosulfur polymer composites(STIs) are developed.Relationship between the structure and the electrochemical conversion behavior of STIs is systematically investigated.It is found that the structure of STIs varies with the synthetic temperature,and correspondingly the electrochemical redox of sulfur can be controlled from conventional "solid-liquid-solid" conversion to the "solid-solid" one.Among the STI series,the STI-5 composite realizes an ideal solid-phase conversion and demonstrates great potential for building a Li-S battery with high-energy density and long-cyclelife:it realizes stable cycling over 1000 cycles in carbonate electrolyte,with a degradation rate of0.053% per cycle;the corresponding pouch cell shows almost no capacity decay for 125 cycles under the conditions of high sulfur loading(4.5 mg cm^(-2)) and lean electrolyte(8 μL mg_s^(-1)).In addition,the tailoring strategy of STI can also apply to other precursors with allyl functional groups to develop new organosulfur polymers for "solid-solid" sulfur cathodes.The vulcanized triallyl phosphate(STP) and triallylamine(STA) both show great lithium storage potential.This strategy successfully develops a new family of organosulfur polymers as cathodes for Li-S batteries via solid-phase conversion of sulfur,and brings insights to the mechanism study in Li-S batteries.

关键词： Organosulfur polymer lithium–sulfur batteries Allyl functional groups Reaction mechanism Solid–solid conversion

Guanine-assisted N-doped ordered mesoporous carbons as efficient capacity decaying suppression materials for lithium–sulfur batteries

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Journal of Materials Science & Technology 2022年第6期101卷 155-164页

作者： Riguang Cheng Yanxun Guan Yumei Luo Chenchen Zhang Yongpeng Xia Sheng Wei Mengmeng Zhao Qi Lin Hao Li Shiyou Zheng Federico Rosei Lixian Sun Fen Xu Hongge Pan School of Material Science&Engineering Guangxi Key Laboratory of Information Materials and Guangxi Collaborative Innovation Center of Structure and Property for New Energy and MaterialsGuilin University of Electronic TechnologyGuilin 541004China School of Mechanical&Electrical Engineering Guilin University of Electronic TechnologyGuilin 541004China School of Material Science&Engineering University of Shanghai for Science&TechnologyShanghai 200093China CentreÉnergie Matériaux et TélécommunicationsInstitut National de la Recherche Scientifique1650 Boul.Lionel BouletVarennesJ3×1S2QuébecCanada School of New Energy Science and Technology Xi’an Technological UniversityChina

lithium–sulfur(Li–S)batteries are considered promising next-generation energy storage devices due to their high weight capacities and theoretical energy densities,which are significantly higher than those of conventional lithium-ion batteries.However,the sulfur cathode presents two major drawbacks,specifically low specific capacity caused by the poor electrical conductivities of the active materials and fast capacity decay caused by polysulfide dissolution/shuttling.Herein,a high-rate and high-stability dendritic material consisting of N-doped ordered mesoporous carbons(NOMCs)was successfully synthesized via a facile and low-cost calcination method.The highly ordered mesoporous carbon skeleton limited the growth of the sulfur nanofiller within its channels and provided the necessary electrical contact with the insulating sulfur.Furthermore,N-doped heteroatoms presented strong binding sites for trapping polysulfide intermediates,achieving high electrochemical activity,which promoted polysulfide conversion reactions.As a result,the prepared NOMC-2/S cathode material with 1.2-1.5 mg cm^(-2)of sulfur displayed excellent electrochemical performance with a high-rate capability of 460.5 m Ah g^(-1)at 1 C,a high specific capacity of 530.9 m Ah g^(-1)after 200 cycles at 0.1 C,and a decay rate of~0.19%per cycle.

关键词： lithium–sulfur batteries N-doped ordered mesoporous carbons Electrochemistry

High-Entropy Alloys to Activate the sulfur Cathode for lithium-sulfur batteries

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Energy & Environmental Materials 2023年第3期6卷 40-49页

作者： Zhenyu Wang Hailun Ge 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

sulfur element possesses an ultrahigh theoretical specific capacity,while the utilization of sulfur in the whole cathode is lower obviously owing to the sluggish kinetics of sulfur and discharged products,limiting the enhancement on energy density of lithium-sulfur batteries.Herein,for the first time,Fe_(0.24)Co_(0.26)Ni_(0.10)Cu_(0.15)Mn_(0.25)high-entropy alloy is introduced as the core catalytic host to activate the electrochemical performance of the sulfur cathode for lithium-sulfur batteries.It is manifested that Fe_(0.24)Co_(0.26)Ni_(0.10)Cu_(0.15)Mn_(0.25)high-entropy alloy nanocrystallites distributed on nitrogen-doped carbon exhibit high electrocatalytic activity toward the conversion of solid sulfur to solid discharged products across soluble intermediate lithium polysulfides.In particular,benefiting from the accelerated kinetics by high-entropy alloy nanocrystallites and synergistic adsorption by nitrogen-doped carbon,the cathode exhibits high reversible capacity of 1079.5 mAh g_(-cathode)^(-1)(high utilization of 89.4%)with the whole cathode as active material,instead of sulfur element.Moreover,under both lean electrolyte(3μmg^(-1))and ultrahigh sulfur loading(27.0 mg cm^(-2))condition,the high discharge capacity of 868.2 mAh g_(-cathode)^(-1)can be still achieved for the sulfur cathode.This strategy opens up a new path to explore catalytic host materials for enhancing the utilization of sulfur in the whole cathode for lithium-sulfur batteries.

关键词： catalytic host electrochemical performance high-entropy alloy lithium–sulfur batteries sulfur cathode

High-valence sulfur-containing species in solid electrolyte interphase stabilizes lithium metal anodes in lithium–sulfur batteries

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Journal of Energy Chemistry 2022年第5期31卷 300-305页

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

The interfacial stability of lithium metal anodes dictated by solid electrolyte interphase(SEI) is essential for long-cycling high-energy-density lithium–sulfur batteries. Nevertheless, critical components of SEI for interfacial stabilization are particularly indistinct. Herein, the effect of various sulfur-containing components in SEI for stabilizing lithium metal anodes is disclosed in lithium–sulfur batteries. High-valence sulfur-containing species(Li_(2)SO_(3) and Li_(2)SO_(4)) in SEI are conducive to uniform lithium deposition and stabilizing lithium metal anodes. In contrast, low-valence sulfur-containing species(Li_(2)S_(3) and Li_(2)S_(4)) in SEI result in aggressive lithium dendrites and dead lithium. This work identifies the role of sulfurcontaining components in SEI for stabilizing lithium metal anodes and provides rational design principles of SEI for protecting lithium metal anodes in practical lithium–sulfur batteries.

关键词： lithium–sulfur batteries lithium anode Solid electrolyte interphase lithium plating Practical conditions

WP Nanocrystals on N,P Dual-Doped Carbon Nanosheets with Deeply Analyzed Catalytic Mechanisms for lithium–sulfur batteries

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CCS Chemistry 2023年第2期5卷 397-411页

作者： Peng Wang Zhengchunyu Zhang Ning Song Xuguang An Jie Liu Jinkui Feng Baojuan Xi Shenglin Xiong School of Chemistry and Chemical Engineering State Key Laboratory of Crystal MaterialsShandong UniversityJinan 250100 School of Mechanical Engineering Chengdu UniversityChengdu 610106 The State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050 School of Materials Science and Engineering Shandong UniversityJinan 250061

The use of transition-metal phosphides(TMPs)as catalytic materials to accelerate kinetics of lithium polysulfide(LiPS)conversion has unique advantages.Nevertheless,simple and low-cost preparation strategies are still required for the synthesis of novel TMPs with satisfactory performance.Importantly,the in-depth understanding of the effect of intrinsic interaction between catalytic materials and LiPSs on the promoted kinetics remains limited.Herein,a novel structure of tungsten phosphide(WP)nanocrystals decorated on N,P codoped carbon sheets(WP/NPC)with uniform dispersion is designed by a structure-oriented strategy to promote LiPS redox kinetics.The electrochemical kinetics measurements coupled with density functional theory computations and in situ/ex situ characterizations demonstrate that the strong interaction through W–S bonding and the favorable interfacial charge state of WP-LiPSs promote the nucleation and dissociation of Li2S.Benefiting from this superiority,the WP/NPG-based lithium–sulfur batteries indicate significantly improved electrochemical performance with good cycling life and excellent rate capability.This work provides a methodology for the design of TMP-involved electrode materials and a fundamental understanding of the intrinsic mechanism of catalysis.

关键词： WP nanocrystals in situ self-phosphating shuttling effect electrocatalysis mechanism lithium–sulfur batteries

Rational design of nanoarray structures for lithium-sulfur batteries:recent advances and future prospects

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Materials Futures

Materials Futures 2023年第4期2卷 53-78页

作者： Longtao Ren Jun Liu Abdul Hameed Pato Yan Wang Xiwen Lu Imran Ali Chandio Mingyue Zhou Wen Liu Haijun Xu Xiaoming Sun College of Chemistry Beijing University of Chemical TechnologyBeijing 100029People’s Republic of China State Key Laboratory of Chemical Resource Engineering Beijing 100029People’s Republic of China Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing 100029People’s Republic of China Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084People’s Republic of China College of Mathematics and Physics Beijing University of Chemical TechnologyBeijing 100029People’s Republic of China

lithium-sulfur(Li-S)batteries are considered as promising candidates for future-generation energy storage systems due to their prominent theoretical energy density.However,their application is still hindered by several critical issues,e.g.,the low conductivity of sulfur species,the shuttling effects of soluble lithium polysulfides,volumetric expansion,sluggish redox kinetics,and uncontrollable Li dendritic formation.Considerable research efforts have been devoted to breaking through the obstacles that are preventing Li-S batteries from realizing practical application.Recently,benefiting from the no additives/binders,buffer of volume change,high sulfur loading and suppression of lithium dendrites,nanoarray(NA)structures have have emerged as efficient and durable electrodes in Li-S batteries.In this work,recent advances in the design,synthesis and application of NA structures in Li-S batteries are reviewed.First,the multifunctional merits and typical synthetic strategies of employing NA structure electrodes for Li-S batteries are outlined.Second,the applications of NA structures in Li-S batteries are discussed comprehensively.Finally,the challenge and rational design of NA structure for Li-S batteries are analyzed in depth,with the aim of providing promising orientations for the commercialization of high-energy-density Li-S batteries.

关键词： nanoarrays electrocatalysts surface and interface engineering lithium–sulfur batteries modulated strategies