Fiber-supercapacitors(FSCs)are promising power sources for miniature portable and wearable electronic devices.However,the development and practical application of these FSCs have been severely hindered by their low vo...Fiber-supercapacitors(FSCs)are promising power sources for miniature portable and wearable electronic devices.However,the development and practical application of these FSCs have been severely hindered by their low volumetric capacitance and narrow operating voltage.In this work,vertically aligned nickel cobalt sulfide(Ni Co2S4)nanowires grown on carbon nanotube(CNT)fibers were achieved through an in-situ two-step hydrothermal reaction method.The as-prepared Ni Co2S4@CNT fiber electrode exhibits a high volumetric capacitance of 2332 F cm-3,benefiting from its superior electric conductivity,large surface area,and rich Faradic redox reaction sites.Furthermore,a Ni Co2S4@CNT//VN@CNT(vanadium nitride nanosheets grown on CNT fibers)asymmetric fiber-supercapacitor(AFSC)was successfully fabricated.The device exhibits an operating voltage up to 1.6 V and a high volumetric energy density of 30.64m Wh cm-3.The device also possesses outstanding flexibility as evidenced by no obvious performance degradation under various bending angles and maintaining high capacitance after 5000 bending cycles.This work promotes the practical application of flexible wearable energy-storage devices.展开更多
Aqueous zinc battery has been regarded as one of the most promising energy storage systems due to its low cost and environmental benignity.However,the safety concern on Zn anodes caused by uncontrolled Zn dendrite gro...Aqueous zinc battery has been regarded as one of the most promising energy storage systems due to its low cost and environmental benignity.However,the safety concern on Zn anodes caused by uncontrolled Zn dendrite growth in aqueous electrolyte hinders their application.Herein,sucrose with multi-hydroxyl groups has been introduced into aqueous electrolyte to modify Zn^(2+)solvation environment and create a protection layer on Zn anode,thus effectively retarding the growth of zinc dendrites.Atomistic simulations and experiments confirm that sucrose molecules can enter into the solvation sheath of Zn^(2+),and the as-formed unique solvation structure enhances the mobility of Zn^(2+).Such fast Zn^(2+)kinetics in sucrose-modified electrolyte can successfully suppress the dendrite growth.With this sucrose-modified aqueous electrolyte,Zn/Zn symmetric cells present more stable cycle performance than those using pure aqueous electrolyte;Zn/C cells also deliver an impressive higher energy density of 129.7 Wh·kg^(−1)and improved stability,suggesting a great potential application of sucrose-modified electrolytes for future Zn batteries.展开更多
A copper-catalyzed 1,1-difunctionalization of terminal alkynes was achieved via a three-component reaction, providing a variety of vinyl sulfones with good yields and excellent chemo-and stereoselectivity. Preliminary...A copper-catalyzed 1,1-difunctionalization of terminal alkynes was achieved via a three-component reaction, providing a variety of vinyl sulfones with good yields and excellent chemo-and stereoselectivity. Preliminary mechanistic studies indicated that the reaction probably underwent a Cu-catalyzed formal C–H insertion to produce an allene intermediate, which was then trapped by a sulfonyl anion to give the corresponding product.展开更多
Low-temperature zinc batteries(LT-ZIBs)based on aqueous electrolytes show great promise for practical applications owing to their natural resource abundance and low cost.However,they suffer from sluggish kinetics with...Low-temperature zinc batteries(LT-ZIBs)based on aqueous electrolytes show great promise for practical applications owing to their natural resource abundance and low cost.However,they suffer from sluggish kinetics with elevated energy barriers due to the dissociation of bulky Zn(H2O)62+solvation structure and free Zn2+diffusion,resulting in unsatisfactory lifespan and performance.Herein,dissimilar to solvation shell tuning or layer spacing enlargement engineering,delocalized electrons in cathode through constructing intrinsic defect engineering is proposed to achieve a rapid electrocatalytic desolvation to obtain free Zn2+for insertion/extraction.As revealed by density functional theory calculations and interfacial spectroscopic characterizations,the intrinsic delocalized electron distribution propels the Zn(H2O)62+dissociation,forming a reversible interphase and facilitating Zn2+diffusion across the electrolyte/cathode interface.The as-fabricated oxygen defect-rich V2O5 on hierarchical porous carbon(ODVO@HPC)electrode exhibits high capacity robustness from 25 to20℃.Operating at-20℃,the ODVO@HPC delivers 191 mAh g-1 at 50 A g-1 and lasts for 50000 cycles at 10 A g-1,significantly enhancing the power density and lifespan under low-temperature environments in comparison to previous reports.Even with areal mass loading of-13 mg cm2,both coin cells and pouch batteries maintain excellent stability and areal capacities,realizing practical high-performance LT-ZIBs.展开更多
α-Synuclein(α-syn)forms structurally distinct fibril polymorphs with various pathological activities in different subtypes of synucleinopathies,such as Parkinson's disease(PD).As a unique proteinaceous polymer,t...α-Synuclein(α-syn)forms structurally distinct fibril polymorphs with various pathological activities in different subtypes of synucleinopathies,such as Parkinson's disease(PD).As a unique proteinaceous polymer,the mechanical property ofα-syn fibril is a primary determinant of its neurotoxicity,immunogenicity,and seeding and transmission capacity.Nevertheless,how genetic mutations inα-syn fibrils cause varied polymer behaviors remains largely unknown.Using optical tweezers,we quantitatively characterize the mechanical properties of threeα-syn fibril variants at the single-molecule level.We find that wild-typeα-syn fibrils are generally more sustainable to an axial disruption force than those formed by the disease-causing E46K and A53Tα-syn mutants,whereas their heterogeneous elastic properties manifest similarity.Based on the molecular dynamics simulations,theβ-sheet motif and the interface between the two protofilaments dominate in stabilizing the fibril structure.Additionally,single-molecule and simulation analysis consistently reveal the force-drivenα-syn protein unfolding without a fibril break.Due to the flexible periphery,these subtle structural changes become more pronounced with the E46K fibril.The structure–mechanics relationship ofα-syn fibrils built in this work sheds new light on the fibril assembly and disassembly mechanism and the mutant-associated pathogenesis in PD.展开更多
基金funding support from the CASQueensland Collaborative Science Fund(121E32KYSB20160032)the National Natural Science Foundation of China(No.21403287,No.21433013,51402345,21773291)+1 种基金the National Key R&D Program of China(2016YFB0100100)the CAS-DOE Joint Research Program(121E32KYSB20150004)。
文摘Fiber-supercapacitors(FSCs)are promising power sources for miniature portable and wearable electronic devices.However,the development and practical application of these FSCs have been severely hindered by their low volumetric capacitance and narrow operating voltage.In this work,vertically aligned nickel cobalt sulfide(Ni Co2S4)nanowires grown on carbon nanotube(CNT)fibers were achieved through an in-situ two-step hydrothermal reaction method.The as-prepared Ni Co2S4@CNT fiber electrode exhibits a high volumetric capacitance of 2332 F cm-3,benefiting from its superior electric conductivity,large surface area,and rich Faradic redox reaction sites.Furthermore,a Ni Co2S4@CNT//VN@CNT(vanadium nitride nanosheets grown on CNT fibers)asymmetric fiber-supercapacitor(AFSC)was successfully fabricated.The device exhibits an operating voltage up to 1.6 V and a high volumetric energy density of 30.64m Wh cm-3.The device also possesses outstanding flexibility as evidenced by no obvious performance degradation under various bending angles and maintaining high capacitance after 5000 bending cycles.This work promotes the practical application of flexible wearable energy-storage devices.
基金support from the National Natural Science Foundation of China(Nos.22075313 and 21975281)the National Key Research and Development Program of China(No.2020YFB1312902)+3 种基金the Science and Technology Project of Jiangxi Province(No.20192BCD40017)Outstanding Youth Fund of Jiangxi Province(No.20192BCB23028)Jiangxi Double Thousand Talent Program(No.JXSQ2019101072)Science Technology Major Project of Nanchang(No.2020BI47)is acknowledged.
文摘Aqueous zinc battery has been regarded as one of the most promising energy storage systems due to its low cost and environmental benignity.However,the safety concern on Zn anodes caused by uncontrolled Zn dendrite growth in aqueous electrolyte hinders their application.Herein,sucrose with multi-hydroxyl groups has been introduced into aqueous electrolyte to modify Zn^(2+)solvation environment and create a protection layer on Zn anode,thus effectively retarding the growth of zinc dendrites.Atomistic simulations and experiments confirm that sucrose molecules can enter into the solvation sheath of Zn^(2+),and the as-formed unique solvation structure enhances the mobility of Zn^(2+).Such fast Zn^(2+)kinetics in sucrose-modified electrolyte can successfully suppress the dendrite growth.With this sucrose-modified aqueous electrolyte,Zn/Zn symmetric cells present more stable cycle performance than those using pure aqueous electrolyte;Zn/C cells also deliver an impressive higher energy density of 129.7 Wh·kg^(−1)and improved stability,suggesting a great potential application of sucrose-modified electrolytes for future Zn batteries.
基金supported by the National Natural Science Foundation of China(21432009,21672200,21472177,21772185,21801233)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB20000000)
文摘A copper-catalyzed 1,1-difunctionalization of terminal alkynes was achieved via a three-component reaction, providing a variety of vinyl sulfones with good yields and excellent chemo-and stereoselectivity. Preliminary mechanistic studies indicated that the reaction probably underwent a Cu-catalyzed formal C–H insertion to produce an allene intermediate, which was then trapped by a sulfonyl anion to give the corresponding product.
基金the National Key R&D Program of China(2021YFA1201503)National Natural Science Foundation of China(Nos.21972164,22279161,12264038,22309144)+7 种基金the Natural Science Foundation of Jiangsu Province(BK.20210130)China Postdoctoral Science Foundation(2023 M732561,2023 M731084)Innovative and Entrepreneurial Doctor in Jiangsu Province(JSSCBS20211428)J.W.and S.P.acknowledge the funding provided by the Alexander von Humboldt Foundation and the basic funding of the Helmholtz AssociationQ.Z.acknowledges the support of HZWTECH for providing computational facilitiesH.A.acknowledges the University of Hong Kong and the Hong Kong Quantum AI Lab Limited,AIR@Inno HK for supporting his fellowshipWe also thank Nano-X,Suzhou Institute of Nano-tech and Nano-bionics,Chinese Academy of Sciences for the material measurement analysisOpen Access funding enabled and organized by Projekt DEAL.
文摘Low-temperature zinc batteries(LT-ZIBs)based on aqueous electrolytes show great promise for practical applications owing to their natural resource abundance and low cost.However,they suffer from sluggish kinetics with elevated energy barriers due to the dissociation of bulky Zn(H2O)62+solvation structure and free Zn2+diffusion,resulting in unsatisfactory lifespan and performance.Herein,dissimilar to solvation shell tuning or layer spacing enlargement engineering,delocalized electrons in cathode through constructing intrinsic defect engineering is proposed to achieve a rapid electrocatalytic desolvation to obtain free Zn2+for insertion/extraction.As revealed by density functional theory calculations and interfacial spectroscopic characterizations,the intrinsic delocalized electron distribution propels the Zn(H2O)62+dissociation,forming a reversible interphase and facilitating Zn2+diffusion across the electrolyte/cathode interface.The as-fabricated oxygen defect-rich V2O5 on hierarchical porous carbon(ODVO@HPC)electrode exhibits high capacity robustness from 25 to20℃.Operating at-20℃,the ODVO@HPC delivers 191 mAh g-1 at 50 A g-1 and lasts for 50000 cycles at 10 A g-1,significantly enhancing the power density and lifespan under low-temperature environments in comparison to previous reports.Even with areal mass loading of-13 mg cm2,both coin cells and pouch batteries maintain excellent stability and areal capacities,realizing practical high-performance LT-ZIBs.
基金supported by the ShanghaiTech University School of Life Science and Technology Development Fund(SLST-YS2024004 to B.S.)the National Natural Science Foundation of China(32271505 and 32471508 to B.S.,32100993 to L.B.,32090040 to Z.H.,82188101,22425704 and 32171236 to C.L.,32494764,92353302 and 32170683 to D.L.)+4 种基金National Key R&D Program of China(2022YFA1303100 to Z.H.)the Science and Technology Commission of Shanghai Municipality(STCSM)(22ZR1441900 and 23ZR1442200 to B.S.,20XD1425000 and 22JC1410400 to C.L.)the Shanghai Pilot Program for Basic Research-Chinese Academy of Science,Shanghai Branch(CYJ-SHFY-2022-005 to C.L.)the CAS Project for Young Scientists in Basic Research(YSBR-095 to C.L.)Shanghai Basic Research Pioneer Project to C.L.,the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB1040000 and XDB1060000 to C.L.,XDB0450402 to Z.H.).
文摘α-Synuclein(α-syn)forms structurally distinct fibril polymorphs with various pathological activities in different subtypes of synucleinopathies,such as Parkinson's disease(PD).As a unique proteinaceous polymer,the mechanical property ofα-syn fibril is a primary determinant of its neurotoxicity,immunogenicity,and seeding and transmission capacity.Nevertheless,how genetic mutations inα-syn fibrils cause varied polymer behaviors remains largely unknown.Using optical tweezers,we quantitatively characterize the mechanical properties of threeα-syn fibril variants at the single-molecule level.We find that wild-typeα-syn fibrils are generally more sustainable to an axial disruption force than those formed by the disease-causing E46K and A53Tα-syn mutants,whereas their heterogeneous elastic properties manifest similarity.Based on the molecular dynamics simulations,theβ-sheet motif and the interface between the two protofilaments dominate in stabilizing the fibril structure.Additionally,single-molecule and simulation analysis consistently reveal the force-drivenα-syn protein unfolding without a fibril break.Due to the flexible periphery,these subtle structural changes become more pronounced with the E46K fibril.The structure–mechanics relationship ofα-syn fibrils built in this work sheds new light on the fibril assembly and disassembly mechanism and the mutant-associated pathogenesis in PD.
