Despite the intriguing merits of lithium-sulfur(Li-S) systems, they still suffer from the notorious‘‘shuttling-effect" of polysulfides. Herein, carbon materials with rational tailoring of morphology and pores w...Despite the intriguing merits of lithium-sulfur(Li-S) systems, they still suffer from the notorious‘‘shuttling-effect" of polysulfides. Herein, carbon materials with rational tailoring of morphology and pores were designed for strong loading/adsorption with the controlling of energy-storage ability.Through rational tailoring, it is strongly verified that such engineering of evolutions result in variational of sulfur immobilization in the obtained carbon. As expected, the targeted sample delivers a stable capacity of 925 m Ah g^(-1) after 100 loops. Supporting by the "cutting-off" manners, it is disclosed that mesopores in carbon possess more fascinated traits than micro/macropores in improving the utilization of sulfur and restraining Li_(2)S_x(4≤x≤8). Moreover, the long-chain polysulfide could be further consolidated by auto-doping oxygen groups. Supported by in-depth kinetic analysis, it is confirmed that the kinetics of ion/e-transfer during charging and discharging could be accelerated by mesopores, especially in stages of the formation of solid S_(8) and Li_(2)S, further improving the capacity of ion-storage in Li-S battery. Given this, the elaborate study provide significant insights into the effect of pore structure on kinetic performance about Li-storage behaviors in Li-S battery, and give guidance for improving sulfur immobilization.展开更多
Hydrogen sulfide(H_(2)S)is an industrial exhausted gas that is highly toxic to humans and the environment.Combining desulfurization and fabrication of cathode materials for lithium-sulfur batteries(LSBs)can solve this...Hydrogen sulfide(H_(2)S)is an industrial exhausted gas that is highly toxic to humans and the environment.Combining desulfurization and fabrication of cathode materials for lithium-sulfur batteries(LSBs)can solve this issue with a double benefit.Herein,the amino-functionalized lotus root-like carbon nanofibers(NH_(2)-PLCNFs)are prepared by the amination of electrospinning carbon nanofibers under dielectric barrier discharge plasma.Selective catalytic oxidation of H_(2)S to elemental sulfur(S)is achieved over the metalfree NH_(2)-PLCNFs catalyst,and the obtained composite S@NH_(2)-PLCNFs is further used as cathode in LSBs.NH_(2)-PLCNFs enable efficient desulfurization(removal capacity as high as 3.46 g H_(2)S g^(−1) catalyst)and strongly covalent stabilization of S on modified carbon nanofibers.LSBs equipped with S@NH_(2)-PLCNFs deliver a high specific capacity of 705.8 mA h g^(−1) at 1 C after 1000 cycles based on the spatial confinement and the covalent stabilization of electroactive materials on amino-functionalized porous carbon matrix.It is revealed that S@NH_(2)-PLCNFs obtained by this kind of chemical vapor deposition leads to a more homogeneous S distribution and superior electrochemical performance to the sample S/NH_(2)-PLCNF-M prepared by the traditional molten infusion.This work opens a new avenue for the combination of environment protection and energy storage.展开更多
Resulting from the development of electric vehicles,high energy-density Li-S batteries have recently attracted ever-increasing attentions worldwide.However,continuous dissolution of cathodic sulfur and followed shuttl...Resulting from the development of electric vehicles,high energy-density Li-S batteries have recently attracted ever-increasing attentions worldwide.However,continuous dissolution of cathodic sulfur and followed shuttle effect of polysulfides lead to very limited service lifetime for currently-applied Li-S batteries.Herein,a 3 D porous graphene aerogel(GA)decorated with high exposure of anatase TiO2(001)nanoplatelets is proposed as robust host to immobilize cathodic sulfur.Compared with commonly used TiO2(101)nanoparticles,the Ti O2(001)nanoplatelets have highly matched lattices with graphene(002)nanosheets,thus facilitating the electronic transfer.The in-site assembled TiO2@GA host exhibits superior sulfur-immobilized capability,which cannot only entrap sulfur by physical confinement,but also capture dissoluble sulfurous species by chemical bonding.The fabricated S@TiO2@GA cathode shows excellent electrochemical performance with high discharge capacity,superior rate capability,and durable cycling stability as well,supposed to be a promising cathode for high-performance Li-S battery applications.展开更多
The ’shuttle effect’ of polysulfide causing rapid capacity fade and low coulo mbic efficiency of high ene rgy storage lithium-sulfur(Li-S) batteries.Herein,a sandwich structure of bamboo charcoal/sulfur coating by a...The ’shuttle effect’ of polysulfide causing rapid capacity fade and low coulo mbic efficiency of high ene rgy storage lithium-sulfur(Li-S) batteries.Herein,a sandwich structure of bamboo charcoal/sulfur coating by aluminum fluoride(BC@S@AlF3) composites is designed and fabricated for the first time.The as-designed cathode exhibited excellent electrochemical properties and stable capacity retention.The initial capacity reaches 1119 mA h/g and the capacity after 100 cycles is 869 mA h/g at 0.5 C,which is much stable than that of composite materials without bamboo charcoal or AlF3 coating.Moreover,the BC@S@AlF3 cathode presents excellent long-term capacity stability with a capacity decay of 0.073% per cycle during 500 charge/discharge cycles at 1 C,offering a potential for use in high energy Li-S batteries.The physical confinement,chemical ancho ring,and catalysis conversion for active sulfur are achieved simultaneously with the AlF3 coating and bamboo charcoal core with porous structure.展开更多
基金financially supported by National National Key Research and Development Program of China (2019YFC1907801, 2018YFC1900305, 2018YFC1901601, 2018YFC1901602)the Natural Science Foundation of China (52004334, 51622406, 51634009 and U1704252)+4 种基金National 111 Project (No. B14034)the National Key R&D Program of China (2018YFC1901901)the Collab-orative Innovation Center for Clean and Efficient Utilization of Strategic Metal Mineral Resources, Found of State Key Laboratory of Mineral Processing (BGRIMM-KJSKL-2017-13)the Fundamental Research Funds for the Central Universities of Central South University (2019zzts1712020zzts203)the Hunan Provincial Innovation Foundation for Postgraduate (CX20190227)。
文摘Despite the intriguing merits of lithium-sulfur(Li-S) systems, they still suffer from the notorious‘‘shuttling-effect" of polysulfides. Herein, carbon materials with rational tailoring of morphology and pores were designed for strong loading/adsorption with the controlling of energy-storage ability.Through rational tailoring, it is strongly verified that such engineering of evolutions result in variational of sulfur immobilization in the obtained carbon. As expected, the targeted sample delivers a stable capacity of 925 m Ah g^(-1) after 100 loops. Supporting by the "cutting-off" manners, it is disclosed that mesopores in carbon possess more fascinated traits than micro/macropores in improving the utilization of sulfur and restraining Li_(2)S_x(4≤x≤8). Moreover, the long-chain polysulfide could be further consolidated by auto-doping oxygen groups. Supported by in-depth kinetic analysis, it is confirmed that the kinetics of ion/e-transfer during charging and discharging could be accelerated by mesopores, especially in stages of the formation of solid S_(8) and Li_(2)S, further improving the capacity of ion-storage in Li-S battery. Given this, the elaborate study provide significant insights into the effect of pore structure on kinetic performance about Li-storage behaviors in Li-S battery, and give guidance for improving sulfur immobilization.
基金financial support from projects funded by the National Natural Science Foundation of China(22179017,52172038).
文摘Hydrogen sulfide(H_(2)S)is an industrial exhausted gas that is highly toxic to humans and the environment.Combining desulfurization and fabrication of cathode materials for lithium-sulfur batteries(LSBs)can solve this issue with a double benefit.Herein,the amino-functionalized lotus root-like carbon nanofibers(NH_(2)-PLCNFs)are prepared by the amination of electrospinning carbon nanofibers under dielectric barrier discharge plasma.Selective catalytic oxidation of H_(2)S to elemental sulfur(S)is achieved over the metalfree NH_(2)-PLCNFs catalyst,and the obtained composite S@NH_(2)-PLCNFs is further used as cathode in LSBs.NH_(2)-PLCNFs enable efficient desulfurization(removal capacity as high as 3.46 g H_(2)S g^(−1) catalyst)and strongly covalent stabilization of S on modified carbon nanofibers.LSBs equipped with S@NH_(2)-PLCNFs deliver a high specific capacity of 705.8 mA h g^(−1) at 1 C after 1000 cycles based on the spatial confinement and the covalent stabilization of electroactive materials on amino-functionalized porous carbon matrix.It is revealed that S@NH_(2)-PLCNFs obtained by this kind of chemical vapor deposition leads to a more homogeneous S distribution and superior electrochemical performance to the sample S/NH_(2)-PLCNF-M prepared by the traditional molten infusion.This work opens a new avenue for the combination of environment protection and energy storage.
基金financially supported by the National Key R and D Program of China(No.2019YFA0210300)the Hunan Provincial Natural Science Foundation of China(No.2019JJ40359)+1 种基金the Hunan Provincial S and T Plan of China(Nos.2017TP1001,2016TP1007)the Open-End Fund for the Valuable and Precision Instruments of Central South University(CSUZC2020016)。
文摘Resulting from the development of electric vehicles,high energy-density Li-S batteries have recently attracted ever-increasing attentions worldwide.However,continuous dissolution of cathodic sulfur and followed shuttle effect of polysulfides lead to very limited service lifetime for currently-applied Li-S batteries.Herein,a 3 D porous graphene aerogel(GA)decorated with high exposure of anatase TiO2(001)nanoplatelets is proposed as robust host to immobilize cathodic sulfur.Compared with commonly used TiO2(101)nanoparticles,the Ti O2(001)nanoplatelets have highly matched lattices with graphene(002)nanosheets,thus facilitating the electronic transfer.The in-site assembled TiO2@GA host exhibits superior sulfur-immobilized capability,which cannot only entrap sulfur by physical confinement,but also capture dissoluble sulfurous species by chemical bonding.The fabricated S@TiO2@GA cathode shows excellent electrochemical performance with high discharge capacity,superior rate capability,and durable cycling stability as well,supposed to be a promising cathode for high-performance Li-S battery applications.
基金This work was supported by the National Natural Science Foundation of China(Grant No.11602213)the Natural Science Foundation of Hunan province,China(Grant No.2019JJ50578)。
文摘The ’shuttle effect’ of polysulfide causing rapid capacity fade and low coulo mbic efficiency of high ene rgy storage lithium-sulfur(Li-S) batteries.Herein,a sandwich structure of bamboo charcoal/sulfur coating by aluminum fluoride(BC@S@AlF3) composites is designed and fabricated for the first time.The as-designed cathode exhibited excellent electrochemical properties and stable capacity retention.The initial capacity reaches 1119 mA h/g and the capacity after 100 cycles is 869 mA h/g at 0.5 C,which is much stable than that of composite materials without bamboo charcoal or AlF3 coating.Moreover,the BC@S@AlF3 cathode presents excellent long-term capacity stability with a capacity decay of 0.073% per cycle during 500 charge/discharge cycles at 1 C,offering a potential for use in high energy Li-S batteries.The physical confinement,chemical ancho ring,and catalysis conversion for active sulfur are achieved simultaneously with the AlF3 coating and bamboo charcoal core with porous structure.