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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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Advanced chemical strategies for lithium-sulfur batteries: A review

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Green Energy & Environment 2018年第1期3卷 2-19页

作者： Xiaojing Fan Wenwei Sun Fancheng Meng Aiming Xing Jiehua Liu Future Energy Laboratory School of Materials Science and EngineeringHefei University of Technology

lithium-sulfur(Li-S) battery has been considered as one of the most promising rechargeable batteries among various energy storage devices owing to the attractive ultrahigh theoretical capacity and low cost. However, the performance of Li-S batteries is still far from theoretical prediction because of the inherent insulation of sulfur, shuttling of soluble polysulfides, swelling of cathode volume and the formation of lithium dendrites. Significant efforts have been made to trap polysulfides via physical strategies using carbon based materials, but the interactions between polysulfides and carbon are so weak that the device performance is limited. Chemical strategies provide the relatively complemented routes for improving the batteries' electrochemical properties by introducing strong interactions between functional groups and lithium polysulfides. Therefore, this review mainly discusses the recent advances in chemical absorption for improving the performance of Li-S batteries by introducing functional groups(oxygen, nitrogen, and boron, etc.) and chemical additives(metal, polymers, etc.) to the carbon structures, and how these foreign guests immobilize the dissolved polysulfides.

关键词： lithium-sulfur batteries Chemical reaction lithium polysulfides Functional groups Additives

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MXene and MXene-based materials for lithium-sulfur batteries

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Progress in Natural Science:Materials International 2021年第4期31卷 501-513页

作者： Youquan Zhang Cheng Ma Weitao He Chunxiao Zhang Liangjun Zhou Gao Wang Weifeng Wei State Key Laboratory of Powder Metallurgy Central South University Advanced Research Center Central South University

lithium-sulfur(Li–S) batteries are regarded as potential alternatives to lithium-ion batteries due to their extremely high theoretical energy density. Nevertheless, Li–S batteries still suffer from low coulombic efficiency,low sulfur utilization, and poor cycling life, which hinder their further applications. To obtain ideal Li–S cells,intensive work has been dedicated to improve the conductivity of the electrode, inhibiting the shuttle of lithium polysulfides, and promoting the redox of sulfur. Two-dimensional transition metal carbides, nitrides or carbonitrides, also known as MXenes, attracting significant research interest in Li–S batteries due to their high conductivity, abundant active sites, layered structure and adjustable surface chemistry. In this review, we summarize the partial etching methods of MXenes with different surface terminations, the role of MXenes in Li–S batteries and MXene-based composites designed for Li–S batteries based on interfacial chemistry and interlayer structure. In the end, we also propose the perspectives of MXenes for Li–S batteries.

关键词： MXenes lithium-sulfur batteries Interface chemistry lithium polysulfides Heterojunction

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Promoting the sulfur redox kinetics by mixed organodiselenides in high-energy-density lithium-sulfur batteries

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eScience 2021年第1期1卷 44-52页

作者： Meng Zhao Xi-Yao Li Xiang Chen Bo-Quan Li Stefan Kaskel Qiang Zhang 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 Department of Inorganic Chemistry Technische Universität DresdenBergstr.66Dresden 01069Germany

lithium-sulfur(Li-S)batteries are considered as a highly promising energy storage system due to their ultrahigh theoretical energy density.However,the sluggish kinetics of the complex multi-electron sulfur redox reactions seriously hinders the actual battery performance especially under practical working conditions.Homogeneous redox mediation,through elaborately designing the additive molecules,is an effective approach to promote the sulfur redox kinetics.Herein a promoter of mixed organodiselenides(mixed-Se)is proposed to comprehensively improve the sulfur redox kinetics following the redox comediation principles.Concretely,diphenyl diselenide promotes the liquid-liquid conversion between polysulfides and the solid-liquid conversion regarding lithium sulfide oxidation to polysulfides,while dimethyl diselenide enhances the liquid-solid conversion regarding lithium sulfide deposition.Consequently,the mixed-Se promoter endows a high discharge capacity of 1002 mAh g^(−1)with high sulfur loading of 4.0 mg cm^(−2),a high capacity retention of 81.6%after 200 cycles at 0.5 C,and a high actual energy density of 384 Wh kg^(−1)at 0.025 C in 1.5 Ah-level Li-S pouch cells.This work affords an effective kinetic promoter to construct high-energy-density Li-S batteries and inspires molecular design of kinetic promoters toward targeted energy-related redox reactions.

关键词： lithium-sulfur batteries Sulfur redox kinetics Organodiselenide lithium polysulfides Redox comediation

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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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