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In-situ embedding CoTe catalyst into 1D-2D nitrogen-doped carbon to didirectionally regulate lithium-sulfur batteries

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Nano Research 2022年第10期15卷 8972-8982页

作者： Bin Li Peng Wang Baojuan Xi Ning Song Xuguang An Weihua Chen Jinkui Feng Shenglin Xiong Key Laboratory of Colloid and Interface Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringState Key Laboratory of Crystal MaterialsShandong UniversityJinan 250100China Key Laboratory of Mechanical Engineering of Education School of Mechanical EngineeringChengdu UniversityChengdu 610106China Key Laboratory of Material Processing and Mold of Ministry of Education Zhengzhou UniversityZhengzhou 450001China School of Materials Science and Engineering Shandong UniversityJinan 250061China

Lithium-sulfur(Li-S)batteries have been widely investigated attributed to their advantages of high energy density and cost effectiveness.However,it is still limited by the uncontrolled shuttle effect of the sulfur cathode and the promiscuous dendrite growth over the lithium anode.To handle the above issues,the highly conductive CoTe catalyst is precisely loaded onto nitrogendoped nanotube and graphene-like carbon(CoTe NCGs),which is employed as a bi-functionally integrated host.On the lithium anode,the CoTe NCGs with excellent lithiophilic property effectively regulate the uniform deposition of lithium and achieve the effect of suppressing the disorderly growth of lithium dendrites.On the sulfur cathode,the electrochemical conversion of lithium polysulfides(LiPSs)is catalyzed to mitigate the notorious shuttle effect.In view of the bifunctionality of CoTe NCGs,the assembled full cell can be steadily stable even for 800 cycles at a high rate of 2 C,and the capacity decay rate is only 0.05%per cycle.The areal capacity of 6.0 mAh·cm^(−2) is well retained after 50 cycles under the conditions of high sulfur loading,poor electrolyte(a low electrolyte-to-sulfur ratio,E/S=4.2),and low negative to positive capacity ratio(N/P=1.6:1).

关键词： CoTe nanocrystals dual-functional shuttling effect lithium dendrite Li-S batteries

Structural and chemical engineering of metal-organic framework-derived nickel disulfide nanosheets as the compacted cathode matrix for lithium-sulfur batteries

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Chinese Journal of Structural Chemistry 2023年第9期42卷 34-40页

作者： Qi Zhang Wenxiang Shen Pengyue Li Jinshang Song Lingzhi Zhu Enshan Han Ruihu Wang Xiaoju Li Hebei Key Laboratory of Functional Polymer School of Chemical Engineering and TechnologyHebei University of TechnologyTianjin300130China Fujian Provincial Key Laboratory of Polymer Materials College of Chemistry and Materials ScienceFujian Normal UniversityFuzhou350007China

Lithium-sulfur(Li–S)batteries are recognized as promising high-energy-density storage systems.It is crucial to develop the compacted sulfur cathodes with high sulfur content and high sulfur loading for practical applications.The metal-containing nanosheets are promising cathode matrix to mediate the accompanying problems,such as low sulfur utilization,unavoidable polysulfides shuttling and poor rate performance.Herein,we develop Ni-MOF-based strategy to fabricate nickel disulfide nanosheets on the reduced graphene oxide surface(NSG).Benefiting from nanosheets structure,strong polysulfides affinity,high electronic conductivity and superior electrocatalytic effect of NSG heterostructure,the resultant electrode exhibits high electrochemical performance with 0.021%capacity decay per cycle in 1000 cycles.Remarkably,the electrode with 88 wt%sulfur content and 5.9 mg cm^(−2) sulfur loading delivers reversible capacity of 945 mA h g^(−1),areal capacity of 6.1 mA h cm^(−2) and volumetric capacity of 997 mA h cm^(−3) at 0.5 C,which is comparable with the state-of-the-art those in the reported energy storage systems.This work provides methodology guidance for the development of cathode matrix to achieve high-energy-density and long-life Li–S batteries.

关键词： Lithium-sulfur batteries Metal-organic frameworks Nanosheets Nickel disulfide shuttling effect

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

Increasing sulfur utilization in lithium-sulfur batteries by a Co-MOF-74@MWCNT interlayer

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Journal of Energy Chemistry 2021年第9期30卷 186-193页

作者： SiHyeon Sung Byung Hyuk Kim SeungTaek Lee Sanghyeon Choi Woo Young Yoon Department of Materials Science and Engineering Korea University15GaAnam-dongSungbuk-GuSeoul 136-701Republic of Korea

To improve lithium-sulfur battery performance,Co-MOF-74 has been applied for the first time as an interlayer with multiwalled carbon nanotubes(MWCNTs).Co-MOF-74@MWCNT was synthesized using a solvothermal method.The fabrication of Co-MOF-74@MWCNT was confirmed by scanning electron microscopy,X-ray diffraction,thermogravimetric analysis,and Brunauer-Emmett-Teller testing.The interlayer was fabricated using a filtration method.Assembled batteries were prepared using a CoMOF-74@MWCNT interlayer and an MWCNT interlayer and subsequently investigated via cyclic voltammetry tests.Co-MOF-74 promotes a redox reaction and shows a small peak at 1.85 V.A symmetric and full cell test revealed that the Co-MOF-74@MWCNT cell enables a faster redox reaction and higher capacity than that of the MWCNT cell.After 15 cycles,the Co-MOF-74@MWCNT cell achieved a value of 1112 mAh g^(-1),which is 26% greater than that of the MWCNT cell(880 mAh g^(-1)) at 0.2 C.Voltage profile testing showed that the reason for the higher capacity of the Co-MOF-74@MWCNT cell is that it promotes the conversion of Li_(2)S_(2) to Li_(2)S.Various electrochemical analyses confirmed that the Co-MOF-74@MWCNT interlayer acts not only as a physical and chemical barrier but also promotes the transformation of Li_(2)S_(2) to Li_(2)S.

关键词： Li-S battery shuttling effect Interlayer Sulfur utilization Co-MOF-74

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Hierarchically porous, ultrathin N–doped carbon nanosheets embedded with highly dispersed cobalt nanoparticles as efficient sulfur host for stable lithium–sulfur batteries

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Journal of Energy Chemistry 2020年第11期29卷 106-114页

作者： Mengrui Wang Xunfu Zhou Xin Cai Hongqiang Wang Yueping Fang Xinhua Zhong College of Materials and Energy.South China Agricultural University Guangzhou 510642GuangdongChina Guangdong Laboratory for Lingnan Modem Agriculture South China Agricultural UniversityGuangzhou 510642GuangdongChina Guangxi Key Laboratory of Low Carbon Energy Materials School of Chemistry&Pharmaceutical SciencesGuangxi Normal UniversityGuilin 541004GuangxiChina

The sluggish redox kinetics and shuttle effect of soluble polysulfides intermediate primarily restrict the electrochemical performance of lithium–sulfur(Li–S) batteries. To address this issue, rational design of high–efficiency sulfur host is increasingly demanded to accelerate the polysulfides conversion during charge/discharge process. Herein, we propose a macro–mesoporous sulfur host(Co@NC), which comprises highly dispersed cobalt nanoparticles embedding in N–doped ultrathin carbon nanosheets. Co@NC is simply synthesized via a carbon nitride–derived pyrolysis approach. Owing to the highly conductive graphene–like matrix and well defined porous structure, the designed multifunctional Co@NC host enables rapid electron/ion transport, electrolyte penetration and effective sulfur trapping. More significantly,N heteroatoms and homogeneous Co nanocatalysts in the graphitic carbon nanosheets could serve as chemisorption sites as well as electrocatalytic centers for sulfur species. These Co–N active sites can synergistically facilitate the redox conversion kinetics and mitigate the shuttling of polysulfides, thus leading to improved electrochemical cycling performance of Li–S batteries. As a consequence, the S/Co@NC cathode demonstrates high initial specific capacity(1505 mA h g-1 at 0.1 C) and excellent cycling stability at 1 C over 300 cycles, giving rise to a capacity retention of 91.7% and an average capacity decline of 0.03%cycle-1.

关键词： Rechargeable lithium–sulfur batteries Sulfur host shuttling effect Carbon nanosheets Cobalt nanoparticles Carbon nitride

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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