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Design of ZnSe-CoSe heterostructure decorated in hollow N-doped carbon nanocage with generous adsorption and catalysis sites for the reversibly fast kinetics of polysulfide conversion

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Journal of Energy Chemistry 2023年第11期86卷 135-145,I0004页

作者： Junan Feng Chuan Shi Hanghang Dong Chaoyue Zhang Wendong Liu Yu Liu Tianyi Wang Xiaoxian Zhao Shuangqiang Chen Jianjun Song College of Physics Qingdao UniversityQingdao 266071ShandongChina College of Chemistry and Chemical Engineering Qingdao UniversityQingdao 266071ShandongChina Department of Chemical Engineering School of Environmental and Chemical EngineeringShanghai UniversityShanghai 200444China School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002JiangsuChina Department of Chemistry College of ScienceHebei Agricultural UniversityBaoding 071001HebeiChina

Although lithium-sulfur batteries(Li SBs)are regarded as one of the most promising candidates for the next-generation energy storage system,the actual industrial application is hindered by the sluggish solid–liquid phase conversion kinetics,severe shuttle effect,and low sulfur loadings.Herein,a zeolitic imidazolate framework(ZIF)derived heterogeneous ZnSe-CoSe nanoparticles encapsulated in hollow N-doped carbon nanocage(ZnSe-CoSe-HNC)was designed by etching with tannic acid as a multifunctional electrocatalyst to boost the polysulfide conversion kinetics in LiSBs.The hollow structure in ZIF ensures large inner voids for sulfur and buffering volume expansions.Abundant exposed ZnSe-CoSe heterogeneous interfaces serve as bifunctional adsorption-catalytic centers to accelerate the conversion kinetics and alleviate the shuttle effect.Together with the highly conductive framework,the ZnSe-CoSeHNC/S cathode exhibits a high initial reversible capacity of 1305.3 m A h g-1at 0.2 C,high-rate capability,and reliable cycling stability under high sulfur loading and lean electrolyte(maintaining at 745 m A h g-1after 200 cycles with a high sulfur loading of 6.4 mg cm-2and a low electrolyte/sulfur ratio of 6μL mg^(-1)).Theoretical calculations have demonstrated the heterostructures of ZnSe-CoSe offer higher binding energy to lithium polysulfides than that of ZnSe or CoSe,facilitating the electron transfer to lithium polysulfides.This work provides a novel heterostructure with superior catalytic ability and hollow conductive architecture,paving the way for the practical application of functional sulfur electrodes.

关键词： Lithium-sulfur batteries Heterostructure conversion kinetics Hollow structure Bi-directional catalysis

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Selenium vacancies enable efficient immobilization and bidirectional conversion acceleration of lithium polysulfides for advanced Li-S batteries

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Nano Research 2022年第8期15卷 7234-7246页

作者： Yuanchang Li Zhenfang Zhou Yong Li Zhonghua Zhang Xiaosong Guo Jing Liu Changming Mao Zhenjiang Li Guicun Li College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042China

Heterostructures composed of oxides and sulfides(nitrides or carbides)show great potential as sulfur host additives because of the strong adoptability of oxides and catalytic capability of sulfides towards the notorious lithium polysulfides(LiPSs).However,the migration and conversion pathway of LiPSs is seriously confined at a localized interface with inadequate active sites.In this work,the introduction of selenium vacancies into VSe_(2−x)has been demonstrated to successfully synergize the adsorbability and catalytic reactions of LiPSs at an integrated functional surface.The N-doped carbon nanosheets-assembled flower architectures embedded with selenium vacancy-rich VSe_(2−x)and partial vanadium oxides have been controllably synthesized and employed as the cathode additives for lithium-sulfur(Li-S)batteries.Both the experiments and first-principle calculations reveal their strong adsorption to LiPSs and their bidirectional catalytic functionality towards the conversion between S8 and Li_(2)S.As expected,the charge and discharge kinetics of VSe_(2−x)containing sulfur cathodes is fundamentally improved(an outstanding rate capabilitiy with 693.7 mAh·g^(−1)at 2 C,a remarkable long-term cyclability within 1,000 cycles at 2 C with S loading 2.27 mg·cm^(−2),and an excellent areal capacity with 3.44 mAh·cm^(−2)within 100 cycles at 0.5 C).This work presents an effective resolution to couple the adsorbability and catalytic reactions of LiPSs at the material design perspective,and the insights on bidirectional catalytic functionality are of vital to develop functional materials for advanced Li-S batteries.

关键词： lithium-sulfur batteries selenium vacancies vanadium selenide bidirectional catalysis conversion kinetics

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Terminal sulfur atoms formation via defect engineering strategy to promote the conversion of lithium polysulfides

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Journal of Materials Science & Technology 2022年第8期103卷 221-231页

作者： Yuanchang Li Wenda Li Xiujuan Yan Zhenfang Zhou Xiaosong Guo Jing Liu Changming Mao Zhonghua Zhang Guicun Li College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042China

The defect engineering shows great potential in boosting the conversion of lithium polysulfides intermediates for high energy density lithium-sulfur batteries(LSBs),yet the catalytic mechanisms remain unclear.Herein,the oxygen-defective Li_(4)Ti_(5)O_(12)-xhollow microspheres uniformly encapsulated by N-doped carbon layer(OD-LTO@NC)is delicately designed as an intrinsically polar inorganic sulfur host for the research on the catalytic mechanism.Theoretical simulations have demonstrated that the existence of oxygen deficiencies enhances the adsorption capability of spinel Li_(4)Ti_(5)O_(12)towards soluble lithium polysulfides.Some-S-S-bonds of the Li2S6on the defective Li_(4)Ti_(5)O_(12)surface are fractured by the strong adsorption force,which allows the inert bridging sulfur atoms to be converted into the susceptible terminal sulfur atoms,and reduces the activation energy of the polysulfide conversion in some degree.In addition,with the N-doped carbon layer,secondary hollow microspheres architecture built with primary ultrathin nanosheets provide a large amount of void space and active sites for sulfur storage,adsorption and conversion.The as-designed sulfur host exhibits a remarkable rate capability of 547 m Ah g^(-1)at 4C(1 C=1675 m A g^(-1))and an outstanding long-term cyclability(519 m Ah g^(-1)after 1000 cycles at 3 C).Besides,a high specific capacity of 832 m Ah g^(-1)is delivered even after 100 cycles under a high sulfur mass loading of 3.2 mg cm^(-2),indicating its superior electrochemical performances.This work not only provides a strong proof for the application of oxygen defect in the adsorption and catalytic conversion of lithium polysulfides,but offers a promising avenue to achieve high performance LSBs with the material design concept of incorporating oxygen-deficient spinel structure with hierarchical hollow frameworks.

关键词： Lithium-sulfur batteries Oxygen deficiency Lithium titanate Hierarchical hollow microsphere conversion kinetics

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Oxygen-deficient titanium dioxide supported cobalt nano-dots as efficient cathode material for lithium-sulfur batteries

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Journal of Energy Chemistry 2020年第9期29卷 390-397,I0012页

作者： You Li Xiao Zhang Guihua Liu Ashton Gerhardt Katelyn Evans Aizhong Jia Zisheng Zhang Hebei Provincial Key Laboratory of Green Chemical Technology and High Efficient Energy Saving Tianjin Key Laboratory of Chemical Process SafetySchool of Chemical Engineering and TechnologyHebei University of TechnologyTianjin 300130China Department of Chemical and Biological Engineering University of OttawaOttawaOntario K1N 6N5Canada

Lithium sulfur(Li-S)batteries demonstrate great promise for efficient energy storage systems once the lithium polysulfide(LPS)shuttling and sluggish redox kinetics can be well addressed.Herein,we developed a sea urchin-structured oxygen-deficient titanium dioxide semiconductor anchored with cobalt nano-dots(Co@TiO2-x)as a high-performance multifunctional sulfur host material for Li-S batteries.The sea urchin-structured Co@TiO2-x offers strong structural stability and strengthened chemical interaction towards LPS.Meanwhile,the incorporation of Co nano-dots into TiO2 leads to increased oxygen vacancies,which augments the electrical conduction and benefits LPS conversion acceleration as well.As a result,the oxygen vacancy-rich Co@TiO2-x composite exhibits excellent conductivity,strong LPS confinement and promoted sulfur electrochemical kinetics,rendering enhanced LPS shuttling inhibition and rapid redox reaction.Attributed to these features,the Co@TiO2-x/S cathode exhibits a discharge capacity of 803 mAh g-1at 1 C and a good cyclic stability upon 500 cycles with a low capacity fading rate of 0.07%per cycle.This synergistic design of conductive multifunctional LPS barrier is also promising to enlighten the material engineering in other energy storage applications.

关键词： Titanium dioxide Oxygen vacancy Cobalt nano-dots Lithium-sulfur battery conversion kinetics

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