Zinc-based flow battery is an energy storage technology with good application prospects because of its advantages of abundant raw materials,low cost,and environmental friendliness.The chemical stability of zinc electr...Zinc-based flow battery is an energy storage technology with good application prospects because of its advantages of abundant raw materials,low cost,and environmental friendliness.The chemical stability of zinc electrodes exposed to electrolyte is a very important issue for zinc-based batteries.This paper reports on details of chemical stability of the zinc metal exposed to a series of solutions,as well as the relationship between the morphological evolution of zinc electrodes and their properties in an alkaline medium.Chemical corrosion of zinc electrodes by the electrolyte will change their surface morphology.However,we observed that chemical corrosion is not the main contributor to the evolution of zinc electrode surface morphology,but the main contributor is the Zn/Zn^(2+)electrode process.The morphological evolution of zinc electrodes was controlled by using ionic liquids,1-ethyl-3-methylimidazolium acetate(EMIA),and 1-propylsulfonic-3-methylimidazolium tosylate(PSMIT),and the electrode performance was recorded during the morphological evolution process.It was observed that the reversible change of zinc electrode morphology was accompanied by better electrode performance.展开更多
A novel nano-WS_(2)/graphene nanosheets(GNSs)composite is obtained by ball milling with xylitol as auxiliary agent and hightemperature sintering.Xylitol improves the shear force during ball milling and well overcomes ...A novel nano-WS_(2)/graphene nanosheets(GNSs)composite is obtained by ball milling with xylitol as auxiliary agent and hightemperature sintering.Xylitol improves the shear force during ball milling and well overcomes the van der Waals interactions between the interlayer of graphite and WS_(2).Through high-temperature calcination,GNSs and WS_(2) nanosheets can form tight interface contact.The produced WS_(2)/GNSs composites can be used as anode materials for lithium-ion batteries,while maintaining a high reversible specific capacity of 705 mAh·g^(-1)with the capacity retention of 95%at a current density of 250 mA·g^(-1)after 200 cycles,mainly because WS_(2)/GNSs composites have a higher Li^(+)diffusion coefficient of 2.2×10^(-9)cm^(2)·s^(-1)and a higher specific surface area of 70.10 m^(2)·g^(-1).As a result,the xylitol-assisted ball milling method designed in this work is suitable for extended preparation of peeling of two-dimensional layer materials into nanosheets.展开更多
Fast charging, which aims to shorten recharge times to 10–15 min, is crucial for electric vehicles(EVs),but battery capacity usually decays rapidly if batteries are charged under such severe conditions.Revealing the ...Fast charging, which aims to shorten recharge times to 10–15 min, is crucial for electric vehicles(EVs),but battery capacity usually decays rapidly if batteries are charged under such severe conditions.Revealing the failure mechanism is a prerequisite to improving the charging performance of lithium(Li)-ion batteries. Previous studies have focused less on cathode materials while also mostly focusing on their early changes. Thus, the cumulative effect of long-term fast charging on cathode materials has not been fully studied. Here, we study the changes in a layered cathode material during 1000 cycles of 6 C charging based on 1.6 Ah LiCoO_(2)/graphite pouch cells. Postmortem analysis reveals that the surface structure, charge transfer resistance and Li-ion diffusion coefficient of the cathode degenerate during repeated fast charging, causing a large increase in polarization. This polarization-induced poor utilization of the Li inventory is an important reason for the rapid capacity fading of batteries. These findings deepen the understanding of the aging mechanism for cells undergoing fast charging and can be used as benchmarks for the future development of high-capacity, fast-charging layered cathode materials.展开更多
In this study,a class of rare earth composite sandwich phthalocyanines(MPcs,M=La,Y,Yb,Sc) were prepared and compounded with graphene and carbon nanotubes to obtain MPc/Gr and MPc/CNTs composites.The electrocatalytic b...In this study,a class of rare earth composite sandwich phthalocyanines(MPcs,M=La,Y,Yb,Sc) were prepared and compounded with graphene and carbon nanotubes to obtain MPc/Gr and MPc/CNTs composites.The electrocatalytic behaviors of MPc/Gr and MPc/CNTs electrodes were further investigated.The results show that the central rare earth metal has a large influence on the electrocatalytic performance.For the MPcs/Gr samples,ScPc with the smallest ionic radius and molecular size can be more uniformly dispersed in graphene,and the hydrogen precipitation overpotential of ScPc/Gr electrode is514 mV,corresponding to a Tafel slope of 148 mV/dec,with better electrocatalytic performance than other rare earth metal phthalocyanines.As for the MPc/CNTs composites,LaPc,which has the largest ionic radius and molecular size,is more uniformly dispersed on the surface of CNTs,so that the LaPc/CNT electrode exhibits the best LSV performance with the smallest corresponding Tafel slope(176 mV/dec).The main reason is the different binding modes of MPcs molecules in Gr and CNTs.When rare earth phthalocyanine is combined with layered graphene,the smallest size of rare earth phthalocyanine(ScPc)is more easily embedded in the graphene layer,resulting in better homogeneity of the composite,larger effective contact area and better electrocatalytic performance.In contrast,when rare earth phthalocyanine is bound to carbon nanotubes in a tubular structure,it is mainly bound by attaching to the surface or being entangled by the carbon nanotubes.In this case,the rare-earth phthalocyanine molecules(LaPc)with larger layer spacing can provide more contact area with CNTs,forming a more uniform and effective composite,which eventually provides more active sites and better electrocatalytic performance.展开更多
Four types of sustainable sodium carboxylate- derived materials are investigated as novel electrodes with high performance for lithium-ion batteries. Benefiting from the porous morphology provided by their intermolecu...Four types of sustainable sodium carboxylate- derived materials are investigated as novel electrodes with high performance for lithium-ion batteries. Benefiting from the porous morphology provided by their intermolecular in- teractions, increasing capacity, excellent cycle stability and superior rate performance are observed for the sodium car- boxylate-derived materials. The sodium oxalate (SO) electro- des displayed an increasing discharging capacity at a current density of 50 mA g-1 with maximum values of 242.9 mA h g-1 for SO-631 and 373.9 mA h g-1 for SO-541 during the 100th cycle. In addition, the SO-541, SC-541 (sodium citrate), ST- 541 (sodium tartrate) and SP-541 (sodium pyromellitate) electrode materials displayed high initial capacities of 619.6-392.3, 403.7 and 278.1 mA h g-1, respectively, with capacity retentions of 179%, 148%, 173% and 108%, respectively, after 200 cycles at 50 mA g-1. Even at a high current density of 2,000 mA g-1, the capacities remain 157.6, 131.3, 146.6 and 137.0mAhg-1, respectively. With these superior electro- chemical properties, the sodium carboxylate-derived materials could be considered as promising organic electrode materials for large-scale sustainable lithium-ion batteries.展开更多
Li-rich layered oxide(LLO),e.g.,Li_(1.12)[Mn_(0.56)Ni_(0.16)Co_(0.08)]O_(2)(LRMO),is considered as a promising cathode material due to its superior Li-storage capability.However,the poor cycling stability and large vo...Li-rich layered oxide(LLO),e.g.,Li_(1.12)[Mn_(0.56)Ni_(0.16)Co_(0.08)]O_(2)(LRMO),is considered as a promising cathode material due to its superior Li-storage capability.However,the poor cycling stability and large voltage decay,which are related to the phase transition,limit its industrialization process.Herein,a Mo-doped LRMO(Li_(1.12)[Mn_(0.56)Ni_(0.16)Co_(0.08)]_(0.98)Mo_(0.02)O_(2),LRMO-Mo2.0%)was successfully synthesized via a simple combination of co-precipitation with high-temperature calcination for solving the mentioned above-disadvantages.Compared with the pristine counterpart,the as-prepared LRMO-Mo2.0%shows more excellent electrochemical performance in terms of rate capability(reversible capacity of 118 mA·h·g^(−1) at 5 C),cyclic ability(94.3%capacity retention after 100 cycles at 0.2 C)and discharge midpoint voltage decay(0.11 V after 100 cycles).Systematic investigation of structural evolution and electrochemical kinetics elucidate that the synergic effect of robust oxygen framework and layered/spinel heterostructure is the key to its performance improvement.Such synergy helps to stabilize the layered structure by curbing the structural transformation and oxygen escaping during the electrochemical cycling.This work paved the way for the simple and efficient preparation of highly stable LLO cathode materials.展开更多
基金financially supported by the National Natural Science Foundation of China(Grant Nos.21361010 and 22065014)the National Innovation Training Program(Grant No.202210407024)+1 种基金the Natural Science Foundation of Jiangxi Province(Grant No.20171BAB206001)the Education Department of Jiangxi Province(Grant No.GJJ190433).
文摘Zinc-based flow battery is an energy storage technology with good application prospects because of its advantages of abundant raw materials,low cost,and environmental friendliness.The chemical stability of zinc electrodes exposed to electrolyte is a very important issue for zinc-based batteries.This paper reports on details of chemical stability of the zinc metal exposed to a series of solutions,as well as the relationship between the morphological evolution of zinc electrodes and their properties in an alkaline medium.Chemical corrosion of zinc electrodes by the electrolyte will change their surface morphology.However,we observed that chemical corrosion is not the main contributor to the evolution of zinc electrode surface morphology,but the main contributor is the Zn/Zn^(2+)electrode process.The morphological evolution of zinc electrodes was controlled by using ionic liquids,1-ethyl-3-methylimidazolium acetate(EMIA),and 1-propylsulfonic-3-methylimidazolium tosylate(PSMIT),and the electrode performance was recorded during the morphological evolution process.It was observed that the reversible change of zinc electrode morphology was accompanied by better electrode performance.
基金financially supported by the Education Department of Jiangxi Province (No.GJJ160202,No.GJJ190428)。
文摘A novel nano-WS_(2)/graphene nanosheets(GNSs)composite is obtained by ball milling with xylitol as auxiliary agent and hightemperature sintering.Xylitol improves the shear force during ball milling and well overcomes the van der Waals interactions between the interlayer of graphite and WS_(2).Through high-temperature calcination,GNSs and WS_(2) nanosheets can form tight interface contact.The produced WS_(2)/GNSs composites can be used as anode materials for lithium-ion batteries,while maintaining a high reversible specific capacity of 705 mAh·g^(-1)with the capacity retention of 95%at a current density of 250 mA·g^(-1)after 200 cycles,mainly because WS_(2)/GNSs composites have a higher Li^(+)diffusion coefficient of 2.2×10^(-9)cm^(2)·s^(-1)and a higher specific surface area of 70.10 m^(2)·g^(-1).As a result,the xylitol-assisted ball milling method designed in this work is suitable for extended preparation of peeling of two-dimensional layer materials into nanosheets.
基金supported by the National Natural Science Foundation of China(51874151,51964017)。
文摘Fast charging, which aims to shorten recharge times to 10–15 min, is crucial for electric vehicles(EVs),but battery capacity usually decays rapidly if batteries are charged under such severe conditions.Revealing the failure mechanism is a prerequisite to improving the charging performance of lithium(Li)-ion batteries. Previous studies have focused less on cathode materials while also mostly focusing on their early changes. Thus, the cumulative effect of long-term fast charging on cathode materials has not been fully studied. Here, we study the changes in a layered cathode material during 1000 cycles of 6 C charging based on 1.6 Ah LiCoO_(2)/graphite pouch cells. Postmortem analysis reveals that the surface structure, charge transfer resistance and Li-ion diffusion coefficient of the cathode degenerate during repeated fast charging, causing a large increase in polarization. This polarization-induced poor utilization of the Li inventory is an important reason for the rapid capacity fading of batteries. These findings deepen the understanding of the aging mechanism for cells undergoing fast charging and can be used as benchmarks for the future development of high-capacity, fast-charging layered cathode materials.
基金Project supported by the National Natural Science Foundation of China(21762019)the China Postdoctoral Special Grant Program(2021T140138)+1 种基金Natural Science Foundation of Jiangxi Province(20224ACB204004)Guangdong Yangfan Innovative&Enterpreneurial Research Team Program(2016YT03N101)。
文摘In this study,a class of rare earth composite sandwich phthalocyanines(MPcs,M=La,Y,Yb,Sc) were prepared and compounded with graphene and carbon nanotubes to obtain MPc/Gr and MPc/CNTs composites.The electrocatalytic behaviors of MPc/Gr and MPc/CNTs electrodes were further investigated.The results show that the central rare earth metal has a large influence on the electrocatalytic performance.For the MPcs/Gr samples,ScPc with the smallest ionic radius and molecular size can be more uniformly dispersed in graphene,and the hydrogen precipitation overpotential of ScPc/Gr electrode is514 mV,corresponding to a Tafel slope of 148 mV/dec,with better electrocatalytic performance than other rare earth metal phthalocyanines.As for the MPc/CNTs composites,LaPc,which has the largest ionic radius and molecular size,is more uniformly dispersed on the surface of CNTs,so that the LaPc/CNT electrode exhibits the best LSV performance with the smallest corresponding Tafel slope(176 mV/dec).The main reason is the different binding modes of MPcs molecules in Gr and CNTs.When rare earth phthalocyanine is combined with layered graphene,the smallest size of rare earth phthalocyanine(ScPc)is more easily embedded in the graphene layer,resulting in better homogeneity of the composite,larger effective contact area and better electrocatalytic performance.In contrast,when rare earth phthalocyanine is bound to carbon nanotubes in a tubular structure,it is mainly bound by attaching to the surface or being entangled by the carbon nanotubes.In this case,the rare-earth phthalocyanine molecules(LaPc)with larger layer spacing can provide more contact area with CNTs,forming a more uniform and effective composite,which eventually provides more active sites and better electrocatalytic performance.
基金supported by the National Natural Science Foundation of China (21762019 and 51372104)the Science and Technology Project of Jiangxi Province (20161BAB213082, 20171BAB 206017 and 20151BAB206018)+1 种基金the Science Research Project of Jiangxi Provincial Department of Education (GJJ150672)the College Students Innovation and Entrepreneurship Project (201610407006, and XZG-16-08-17)
文摘Four types of sustainable sodium carboxylate- derived materials are investigated as novel electrodes with high performance for lithium-ion batteries. Benefiting from the porous morphology provided by their intermolecular in- teractions, increasing capacity, excellent cycle stability and superior rate performance are observed for the sodium car- boxylate-derived materials. The sodium oxalate (SO) electro- des displayed an increasing discharging capacity at a current density of 50 mA g-1 with maximum values of 242.9 mA h g-1 for SO-631 and 373.9 mA h g-1 for SO-541 during the 100th cycle. In addition, the SO-541, SC-541 (sodium citrate), ST- 541 (sodium tartrate) and SP-541 (sodium pyromellitate) electrode materials displayed high initial capacities of 619.6-392.3, 403.7 and 278.1 mA h g-1, respectively, with capacity retentions of 179%, 148%, 173% and 108%, respectively, after 200 cycles at 50 mA g-1. Even at a high current density of 2,000 mA g-1, the capacities remain 157.6, 131.3, 146.6 and 137.0mAhg-1, respectively. With these superior electro- chemical properties, the sodium carboxylate-derived materials could be considered as promising organic electrode materials for large-scale sustainable lithium-ion batteries.
基金This work was supported by the National Natural Science Foundation of China(Grant No.51964017,Grant No.51874151)the Jiangxi Provincial Natural Science Foundation(Grant No.20212BAB214004)+1 种基金the Jiangxi Provincial Education Office Natural Science Fund Project(Grant No.GJJ201413)the Jiangxi University of Science and Technology College Student Innovation and Entrepreneurship Training Program Support Project(Grant No.DC2019-042).
文摘Li-rich layered oxide(LLO),e.g.,Li_(1.12)[Mn_(0.56)Ni_(0.16)Co_(0.08)]O_(2)(LRMO),is considered as a promising cathode material due to its superior Li-storage capability.However,the poor cycling stability and large voltage decay,which are related to the phase transition,limit its industrialization process.Herein,a Mo-doped LRMO(Li_(1.12)[Mn_(0.56)Ni_(0.16)Co_(0.08)]_(0.98)Mo_(0.02)O_(2),LRMO-Mo2.0%)was successfully synthesized via a simple combination of co-precipitation with high-temperature calcination for solving the mentioned above-disadvantages.Compared with the pristine counterpart,the as-prepared LRMO-Mo2.0%shows more excellent electrochemical performance in terms of rate capability(reversible capacity of 118 mA·h·g^(−1) at 5 C),cyclic ability(94.3%capacity retention after 100 cycles at 0.2 C)and discharge midpoint voltage decay(0.11 V after 100 cycles).Systematic investigation of structural evolution and electrochemical kinetics elucidate that the synergic effect of robust oxygen framework and layered/spinel heterostructure is the key to its performance improvement.Such synergy helps to stabilize the layered structure by curbing the structural transformation and oxygen escaping during the electrochemical cycling.This work paved the way for the simple and efficient preparation of highly stable LLO cathode materials.