Commercial application of lithium-sulfur(Li-S) batteries is hindered by the insulating nature of sulfur and the dissolution of polysulfides. Here, a bioinspired 3D urchin-like N-doped Murray's carbon nanostructure...Commercial application of lithium-sulfur(Li-S) batteries is hindered by the insulating nature of sulfur and the dissolution of polysulfides. Here, a bioinspired 3D urchin-like N-doped Murray's carbon nanostructure(N-MCN) with interconnected micro-meso-macroporous structure and a polydopamine protection shell has been designed as an effective sulfur host for high-performance Li-S batteries. The advanced 3D hierarchically porous framework with the characteristics of the generalized Murray's law largely improves electrolyte diffusion, facilitates electrons/ions transfer and provides strong chemisorption for active species, leading to the synergistic structural and chemical confinement of polysulfides. As a result,the obtained P@S/N-MCN electrode with high areal sulfur loading demonstrates high capacity at high current densities after long cycles. This work reveals that following the generalized Murray's law is feasible to design high-performance sulfur cathode materials for potentially practical Li-S battery applications.展开更多
Lithium-sulfur(Li-S)batteries have attracted significant attention for their high specific capacity,non-toxic and harmless advantages.However,the shuttle effect limits their development.In this work,small-sized tin di...Lithium-sulfur(Li-S)batteries have attracted significant attention for their high specific capacity,non-toxic and harmless advantages.However,the shuttle effect limits their development.In this work,small-sized tin disulfide(SnS_(2))nanoparticles are embedded between interlayers of twodimensional porous carbon nanosheets(PCNs),forming a multi-functional nanocomposite(PCN-SnS_(2))as a cathode carrier for Li-S batteries.The graphitized carbon nanosheets improve the overall conductivity of the electrode,and the abundant pores not only facilitate ion transfer and electrolyte permeation,but also buffer the volume change during the charge and discharge process to ensure the integrity of the electrode material.More importantly,the physical confinement of PCN,as well as the strong chemical adsorption and catalytic reaction of small SnS_(2)nanoparticles,synergistically reduce the shuttle effect of polysulfides.The interaction between a porous layered structure and physical-chemical confinement gives the PCN-SnS_(2)-S electrode high electrochemical performance.Even at a high rate of 2 C,a discharge capacity of 650 mA h g^(-1)is maintained after 150 cycles,underscoring the positive results of SnS_(2)-based materials for Li-S batteries.The galvanostatic intermittent titration technique results further confirm that the PCN-SnS_(2)-S electrode has a high Li+transmission rate,which reduces the activation barrier and improves the electrochemical reaction kinetics.This work provides strong evidence that reducing the size of SnS_(2)nanostructures is beneficial for capturing and reacting with polysulfides to alleviate their shuttle effect in Li-S batteries.展开更多
Developing anatase/rutile phase-junction in Ti O_(2)to construct Z-scheme system is quite effective to improve its photoelectrochemical activity.In this work,the anatase/rutile phase-junction Ag/Ti O_(2)nanocomposites...Developing anatase/rutile phase-junction in Ti O_(2)to construct Z-scheme system is quite effective to improve its photoelectrochemical activity.In this work,the anatase/rutile phase-junction Ag/Ti O_(2)nanocomposites are developed as photocathodes for hydrogen production.The optimized Ag/Ti O_(2)nanocomposite achieves a high current density of 1.28 m A cm-2,an incident photon-to-current conversion efficiency(IPCE)of 10.8%,an applied bias photon-to-current efficiency(ABPE)of 0.32 at 390 nm and a charge carriers’lifetime up to 2000 s.Such enhancement on photoelectrochemical activity can be attributed to:(ⅰ)the generated Z-scheme system in the anatase/rutile phase-junction Ag/Ti O_(2)photocathode enhances the separation,diffusion and transformation of electron/hole pairs inside the structure,(ⅱ)Ag nanodots modification in the anatase/rutile phases leading to the tuned band gap with enhanced light absorption and(ⅲ)the formed Schottky barrier after Ag nanodots surface modification provides enough electron traps to avoid the recombination of photogenerated electrons and holes.Our results here suggest that developing phase-junction nanocomposite as photocathode will provide a new vision for their enhanced photoelectrochemical generation of hydrogen.展开更多
基金financially supported by National Key Research and Development Program of China [2016YFA0202602, 2021YFE0115800]National Natural Science Foundation of China [22275142, U22B6011, U20A20122, 21671155]+4 种基金Program of Introducing Talents of Discipline to Universities-Plan 111 from the Ministry of Science and Technology and the Ministry of Education of China [Grant No. B20002]Sinopec Ministry of Science and Technology Basic Prospective Research Project [218025-9]Natural Science Foundation of Hubei Province [2021CFB082]Scientific Research Foundation of Wuhan Institute of Technology [K2021042]the Open Key Fund Project of State Key Laboratory of Advanced Technology for Materials Synthesis and Processing [Wuhan University of Technology, 2022-KF-10]。
文摘Commercial application of lithium-sulfur(Li-S) batteries is hindered by the insulating nature of sulfur and the dissolution of polysulfides. Here, a bioinspired 3D urchin-like N-doped Murray's carbon nanostructure(N-MCN) with interconnected micro-meso-macroporous structure and a polydopamine protection shell has been designed as an effective sulfur host for high-performance Li-S batteries. The advanced 3D hierarchically porous framework with the characteristics of the generalized Murray's law largely improves electrolyte diffusion, facilitates electrons/ions transfer and provides strong chemisorption for active species, leading to the synergistic structural and chemical confinement of polysulfides. As a result,the obtained P@S/N-MCN electrode with high areal sulfur loading demonstrates high capacity at high current densities after long cycles. This work reveals that following the generalized Murray's law is feasible to design high-performance sulfur cathode materials for potentially practical Li-S battery applications.
基金the National Key R&D Program of China(2016YFA0202602)the National Natural Science Foundation of China(U1663225)+3 种基金the Fundamental Research Funds for the Central Universities(2020-YB-009)the Academy of Scientific Research and Technology(6611,ASRT,Egypt)the 111 National project(B20002)from the Ministry of Science and Technology and the Ministry of Education,ChinaSinopec Ministry of Science and Technology Basic Prospective Research Project(217027-5 and 218025-9)。
文摘Lithium-sulfur(Li-S)batteries have attracted significant attention for their high specific capacity,non-toxic and harmless advantages.However,the shuttle effect limits their development.In this work,small-sized tin disulfide(SnS_(2))nanoparticles are embedded between interlayers of twodimensional porous carbon nanosheets(PCNs),forming a multi-functional nanocomposite(PCN-SnS_(2))as a cathode carrier for Li-S batteries.The graphitized carbon nanosheets improve the overall conductivity of the electrode,and the abundant pores not only facilitate ion transfer and electrolyte permeation,but also buffer the volume change during the charge and discharge process to ensure the integrity of the electrode material.More importantly,the physical confinement of PCN,as well as the strong chemical adsorption and catalytic reaction of small SnS_(2)nanoparticles,synergistically reduce the shuttle effect of polysulfides.The interaction between a porous layered structure and physical-chemical confinement gives the PCN-SnS_(2)-S electrode high electrochemical performance.Even at a high rate of 2 C,a discharge capacity of 650 mA h g^(-1)is maintained after 150 cycles,underscoring the positive results of SnS_(2)-based materials for Li-S batteries.The galvanostatic intermittent titration technique results further confirm that the PCN-SnS_(2)-S electrode has a high Li+transmission rate,which reduces the activation barrier and improves the electrochemical reaction kinetics.This work provides strong evidence that reducing the size of SnS_(2)nanostructures is beneficial for capturing and reacting with polysulfides to alleviate their shuttle effect in Li-S batteries.
基金supported financially by the Academy of Scientific Research and Technology(No.6618,ASRT,Egypt)the National Key R&D Program of China(No.2016YFA0202602),the National Natural Science Foundation of China(Nos.U1663225 and 21805220)+2 种基金the Fundamental Research Funds for the Central Universities(WUT:Nos.2019Ⅲ012GX and 2020Ⅲ002GX)the Hubei Provincial Natural Science Foundation(No.2018CFB242 and 2020CFB416)supported by the State Key Laboratory of Silicate Materials for Architectures and Center for Materials Research and Analysis at Wuhan University of Technology。
文摘Developing anatase/rutile phase-junction in Ti O_(2)to construct Z-scheme system is quite effective to improve its photoelectrochemical activity.In this work,the anatase/rutile phase-junction Ag/Ti O_(2)nanocomposites are developed as photocathodes for hydrogen production.The optimized Ag/Ti O_(2)nanocomposite achieves a high current density of 1.28 m A cm-2,an incident photon-to-current conversion efficiency(IPCE)of 10.8%,an applied bias photon-to-current efficiency(ABPE)of 0.32 at 390 nm and a charge carriers’lifetime up to 2000 s.Such enhancement on photoelectrochemical activity can be attributed to:(ⅰ)the generated Z-scheme system in the anatase/rutile phase-junction Ag/Ti O_(2)photocathode enhances the separation,diffusion and transformation of electron/hole pairs inside the structure,(ⅱ)Ag nanodots modification in the anatase/rutile phases leading to the tuned band gap with enhanced light absorption and(ⅲ)the formed Schottky barrier after Ag nanodots surface modification provides enough electron traps to avoid the recombination of photogenerated electrons and holes.Our results here suggest that developing phase-junction nanocomposite as photocathode will provide a new vision for their enhanced photoelectrochemical generation of hydrogen.