The shuttle effect caused by soluble lithium polysulfides (LiPSs) deteriorates multiphase transformation reaction kinetics of sulfur species,and gives rise to an unserviceable lithium-sulfur (Li-S) battery.Catalysis,a...The shuttle effect caused by soluble lithium polysulfides (LiPSs) deteriorates multiphase transformation reaction kinetics of sulfur species,and gives rise to an unserviceable lithium-sulfur (Li-S) battery.Catalysis,as a process optimization approach,offers an option to eliminate the intrinsic issues.However,exploring and understanding the role of catalysts on electrode reaction remains critical bottlenecks,particularly as they are prone to continuous evolution under complex dynamic environment.Herein,platinum nanoparticles loaded on MXene nanosheets,as sulfur host,and the action of catalysts on the reaction process are investigated via ex-situ monitors upon solid–liquid–solid chemical transformation of sulfur species.These traces confirm that the high performance originates from electron transfer between catalysts and LiPSs,which lowers the nucleation barrier from liquid LiPSs to solid Li_(2)S/Li_(2)S_(2).Further,the accelerated liquid–solid conversion can alleviate the accumulation of LiPSs,and boost the reaction kinetics in Li-S batteries.The findings corroborate the electronic modulation between catalysts and LiPSs,which is a generalizable strategy to optimize energy conversion efficiency of Li-S batteries.展开更多
The structures of electrode meso-macropore and the solvent polarity are the crucial factors dominating the performance of the electric double layer capacitors(EDLCs),but their impacts are usually tangled and difficult...The structures of electrode meso-macropore and the solvent polarity are the crucial factors dominating the performance of the electric double layer capacitors(EDLCs),but their impacts are usually tangled and difficult to decouple and quantitate.Here the effects of electrode meso-macropore structure and solvent polarity on the specific capacitance of an EDLC are quantitatively investigated using a steady-state continuum model.The simulation results indicate the specific capacitances are significantly affected by the meso-macropore surface structure.The specific capacitances significantly decrease for both convex surface structures but obviously increase for both concave surface structures,with the increase of curvature radius from 1 to 20 nm.As for solvents,the polar solvent with high saturated dielectric permittivity improves the capacitance performance.Moreover,the electrode meso-macropore structure is of more concern compared with solvent polarity when aiming at enhancing the specific capacitance.These results provide fundamentals for the rational design of porous electrodes and polar electrolytes for EDLCs.展开更多
Lithium-Sulfur (Li-S) batteries with high theoretical energy density are promising energy storage systems in the next decades, while the lithium polysulfides (LiPSs) shuttling caused by the sluggish sulfur redox react...Lithium-Sulfur (Li-S) batteries with high theoretical energy density are promising energy storage systems in the next decades, while the lithium polysulfides (LiPSs) shuttling caused by the sluggish sulfur redox reaction severely lowers the practical performance. The use of interlayer between the cathode and separator has been widely investigated to physically or chemically block the LiPSs, while the introduction of catalytic materials is a more effective strategy to accelerate the conversion of LiPSs. MXene with rich surface chemistry has shown its potential for facilitating the catalytic conversion, however, the aggregation of MXene sheets usually leads to the loss of the catalytic active sites. Herein, we report a diatomite/MXene (DE/MX) hybrid material as the bifunctional interlayer for improving the adsorption/conversion of LiPSs in Li-S batteries. The diatomite with porous structure and rich silica-hydroxyl functional groups could trap LiPSs effectively, while prevent the aggregation of MXene. The DE/MX based interlayer showed bifunctions of enhancing the chemical adsorption and promoting the conversion of LiPSs. The Li-S batteries with the DE/MX interlayer delivered an improved cycling stability with a low capacity decay of 0.059% per cycle over 1000 cycles at 1.0 C. Moreover, stable 200 cycles can be realized with a high sulfur loading electrode up to 6.0 mg cm^(−2). This work provides an effective strategy to construct bifunctional interlayers for hindering the shuttling of LiPSs and boosting the practical application of Li-S batteries.展开更多
Polymeric monoliths are of great interest in a variety of applications.A new gelation approach to produce a mechanically stable polystyrene(PS)gel directly from its microemulsion is reported.To produce a PS gel,the as...Polymeric monoliths are of great interest in a variety of applications.A new gelation approach to produce a mechanically stable polystyrene(PS)gel directly from its microemulsion is reported.To produce a PS gel,the as-prepared microemulsion is first demulsified by adding selected watermiscible organic solvents.The small PS latex particles liberated from the surfactant are assembled into a piece of bulk material at an appropriate temperature with a high degree of entanglement of the polymer chains.It is found that the d2 T/ηvalue is an important parameter to evaluate the gelation ability of the organic solvents and helps determine the gelation conditions.Finally,PS monoliths are obtained by capillary drying and their pore structures can be effectively tuned by changing the gelation time and the amount of solvent exchanged with water.This allows the controlled preparation of bulk PS artefacts with densities in the range of 0.06 to 1.14 g cm^(-3).This simple method of PS monolith production avoids the use of shaping tools or chemical templates,needs less energy,and is a promising alternative approach to design either integrated porous or compact polymer materials.展开更多
基金the financial support provided by the National Natural Science Foundation of China (51932005, 22072164, 22025204, 92034301, 21991153 and 22072090)the Liaoning Revitalization Talents Program (XLYC1807175)+2 种基金the Research Fund of Shenyang National Laboratory for Materials Science, the Innovation Program of the Shanghai Municipal Education Commission (2021-01-07-00-02-E00119)the Open Project Program of Key Laboratory of Preparation and Application of Environmental Friendly Materials (Jilin Normal University), Ministry of Education, China (2021002)the Project of Development and Reform Commission of Jilin Provinve (2019C042-1)。
文摘The shuttle effect caused by soluble lithium polysulfides (LiPSs) deteriorates multiphase transformation reaction kinetics of sulfur species,and gives rise to an unserviceable lithium-sulfur (Li-S) battery.Catalysis,as a process optimization approach,offers an option to eliminate the intrinsic issues.However,exploring and understanding the role of catalysts on electrode reaction remains critical bottlenecks,particularly as they are prone to continuous evolution under complex dynamic environment.Herein,platinum nanoparticles loaded on MXene nanosheets,as sulfur host,and the action of catalysts on the reaction process are investigated via ex-situ monitors upon solid–liquid–solid chemical transformation of sulfur species.These traces confirm that the high performance originates from electron transfer between catalysts and LiPSs,which lowers the nucleation barrier from liquid LiPSs to solid Li_(2)S/Li_(2)S_(2).Further,the accelerated liquid–solid conversion can alleviate the accumulation of LiPSs,and boost the reaction kinetics in Li-S batteries.The findings corroborate the electronic modulation between catalysts and LiPSs,which is a generalizable strategy to optimize energy conversion efficiency of Li-S batteries.
基金financially supported by the National Basic Research Program of China(2014CB239702)the National Natural Science Foundation of China(21676082,22008067)the China Postdoctoral Science Foundation(2020M681202,2021T140204)。
文摘The structures of electrode meso-macropore and the solvent polarity are the crucial factors dominating the performance of the electric double layer capacitors(EDLCs),but their impacts are usually tangled and difficult to decouple and quantitate.Here the effects of electrode meso-macropore structure and solvent polarity on the specific capacitance of an EDLC are quantitatively investigated using a steady-state continuum model.The simulation results indicate the specific capacitances are significantly affected by the meso-macropore surface structure.The specific capacitances significantly decrease for both convex surface structures but obviously increase for both concave surface structures,with the increase of curvature radius from 1 to 20 nm.As for solvents,the polar solvent with high saturated dielectric permittivity improves the capacitance performance.Moreover,the electrode meso-macropore structure is of more concern compared with solvent polarity when aiming at enhancing the specific capacitance.These results provide fundamentals for the rational design of porous electrodes and polar electrolytes for EDLCs.
基金The authors appreciate support from the National Key Research and Development Program of China(No.2018YFE0124500)the Young Elite Scientists Sponsorship Program by Tianjin(TJSQNTJ-2020-11)the National Natural Science Foundation of China(Nos.51932005,U1710109).
文摘Lithium-Sulfur (Li-S) batteries with high theoretical energy density are promising energy storage systems in the next decades, while the lithium polysulfides (LiPSs) shuttling caused by the sluggish sulfur redox reaction severely lowers the practical performance. The use of interlayer between the cathode and separator has been widely investigated to physically or chemically block the LiPSs, while the introduction of catalytic materials is a more effective strategy to accelerate the conversion of LiPSs. MXene with rich surface chemistry has shown its potential for facilitating the catalytic conversion, however, the aggregation of MXene sheets usually leads to the loss of the catalytic active sites. Herein, we report a diatomite/MXene (DE/MX) hybrid material as the bifunctional interlayer for improving the adsorption/conversion of LiPSs in Li-S batteries. The diatomite with porous structure and rich silica-hydroxyl functional groups could trap LiPSs effectively, while prevent the aggregation of MXene. The DE/MX based interlayer showed bifunctions of enhancing the chemical adsorption and promoting the conversion of LiPSs. The Li-S batteries with the DE/MX interlayer delivered an improved cycling stability with a low capacity decay of 0.059% per cycle over 1000 cycles at 1.0 C. Moreover, stable 200 cycles can be realized with a high sulfur loading electrode up to 6.0 mg cm^(−2). This work provides an effective strategy to construct bifunctional interlayers for hindering the shuttling of LiPSs and boosting the practical application of Li-S batteries.
基金financially supported by the National Science Fund for Distinguished Young Scholars of China(51525204)the National Natural Science Foundation of China(51702229)。
文摘Polymeric monoliths are of great interest in a variety of applications.A new gelation approach to produce a mechanically stable polystyrene(PS)gel directly from its microemulsion is reported.To produce a PS gel,the as-prepared microemulsion is first demulsified by adding selected watermiscible organic solvents.The small PS latex particles liberated from the surfactant are assembled into a piece of bulk material at an appropriate temperature with a high degree of entanglement of the polymer chains.It is found that the d2 T/ηvalue is an important parameter to evaluate the gelation ability of the organic solvents and helps determine the gelation conditions.Finally,PS monoliths are obtained by capillary drying and their pore structures can be effectively tuned by changing the gelation time and the amount of solvent exchanged with water.This allows the controlled preparation of bulk PS artefacts with densities in the range of 0.06 to 1.14 g cm^(-3).This simple method of PS monolith production avoids the use of shaping tools or chemical templates,needs less energy,and is a promising alternative approach to design either integrated porous or compact polymer materials.
