Sodium-ion batteries are promising candidates for next-generation large-scale energy storage owing to their abundance and low cost.Biphasic intercalation reactions,constrained by kinetic limitations and structural ins...Sodium-ion batteries are promising candidates for next-generation large-scale energy storage owing to their abundance and low cost.Biphasic intercalation reactions,constrained by kinetic limitations and structural instability,fundamentally restrict the rate capability and cycle life of sodium ion batteries.However,precise regulation of these reactions to enhance kinetics remains challenging.Here,we propose a strategy of atomic-scale phase engineering to activate the metastable state and achieve a three-phase reaction through precise Mg^(2+)doping at V sites in Na_(3)V_(2)(PO_(4))_(3).The Mg^(2+)occupancy promotes the exchange between Na1 and Na2 sites,thereby stabilizing a Na_(2)V_(2)(PO_(4))_(3) intermediate.First-principles calculations indicate that Mg^(2+)occupation facilitates charge redistribution by weakening Na-O electrostatic interaction,stabilizing the formation of Na_(2)V_(2)(PO_(4))_(3)phase.The optimized cathode exhibits ultrahigh capacity retention(84.5%after 5000 cycles at 3.51 A g^(-1)),supports ultrafast charging within 120 s,and exceptional rate capability(96.2 mAh g^(-1)at 4.68 A g^(-1)).This work establishes a universal route to unlock hidden reaction pathways by redefining the role of dopants in phase transition control.展开更多
Eradication of MRSA osteomyelitis requires elimination of distinct biofilms.To overcome this,we developed bisphosphonateconjugated sitafloxacin(BCS,BV600072)and hydroxybisphosphonate-conjugate sitafloxacin(HBCS,BV6307...Eradication of MRSA osteomyelitis requires elimination of distinct biofilms.To overcome this,we developed bisphosphonateconjugated sitafloxacin(BCS,BV600072)and hydroxybisphosphonate-conjugate sitafloxacin(HBCS,BV63072),which achieve“target-and-release”drug delivery proximal to the bone infection and have prophylactic efficacy against MRSA static biofilm in vitro and in vivo.Here we evaluated their therapeutic efficacy in a murine 1-stage exchange femoral plate model with bioluminescent MRSA(USA300LAC::lux).Osteomyelitis was confirmed by CFU on the explants and longitudinal bioluminescent imaging(BLI)after debridement and implant exchange surgery on day 7,and mice were randomized into seven groups:1)Baseline(harvested at day7,no treatment);2)HPBP(bisphosphonate control for BCS)+vancomycin;3)HPHBP(hydroxybisphosphonate control for HBCS)+vancomycin;4)vancomycin;5)sitafloxacin;6)BCS+vancomycin;and 7)HBCS+vancomycin.BLI confirmed infection persisted in all groups except for mice treated with BCS or HBCS+vancomycin.Radiology revealed catastrophic femur fractures in all groups except mice treated with BCS or HBCS+vancomycin,which also displayed decreases in peri-implant bone loss,osteoclast numbers,and biofilm.To confirm this,we assessed the efficacy of vancomycin,sitafloxacin,and HBCS monotherapy in a transtibial implant model.The results showed complete lack of vancomycin efficacy while all mice treated with HBCS had evidence of infection control,and some had evidence of osseous integrated septic implants,suggestive of biofilm eradication.Taken together these studies demonstrate that HBCS adjuvant with standard of care debridement and vancomycin therapy has the potential to eradicate MRSA osteomyelitis.展开更多
High capacity Sn_(4)P_(3) is considered as a promising anode candidate for lithium-ion batteries(LIBs),but the fast capacity decay caused by the enormous volume changes and tin agglomeration during cycling largely lim...High capacity Sn_(4)P_(3) is considered as a promising anode candidate for lithium-ion batteries(LIBs),but the fast capacity decay caused by the enormous volume changes and tin agglomeration during cycling largely limits its practical applications.Herein,MWCNTs/Sn_(4)P_(3)@C with a coaxial cable-like structure is designed,where a carbon protective layer is wrapped on the surfaces of Sn_(4)P_(3) nanoparticles to minimize their exposure to the electrolyte and multi-walled carbon nanotubes(MWCNTs)serve as a conductive backbone to disperse Sn_(4)P_(3) nanoparticles.When applied as the lithium container,the MWCNTs/Sn_(4)P_(3)@C composites demonstrate excellent cycling stability(delivering a high reversible capacity of 768.8 mA h g^(-1) after 100 cycles at 100 mA g^(-1) and 569.5 mA h g^(-1) after 1000 cycles at 1000 mA g^(-1))and rate capability(a de-lithiation capacity of 520.1 mA h g^(-1) maintained at a high current density of 2000 mA g^(-1)).Furthermore,full cells composed of the MWCNTs/Sn_(4)P_(3)@C anode and the commercially available LiNi_(1/3)Mn_(1/3)Co_(1/3)O_(2) cathode were also assembled.The result of cycling performance showed a reversible capacity of 507 mA h g^(-1) after 100 cycles,which is far superior to that of bare Sn_(4)P_(3) and MWCNTs/Sn_(4)P_(3) anodes with the reversible capacity lower than 100 mA h g^(-1).These excellent electrochemical performances originate from a synergistic effect between the MWCNT conductive backbone and carbon shell protective layer.The MWCNT backbone can enhance the conductivity and serve as a framework to disperse Sn_(4)P_(3) nanoparticles,thus helping to accommodate the large volume changes during cycling,while the carbon shell not only can further enhance the conductivity but also minimize the side reaction between Sn_(4)P_(3) nanoparticles and electrolytes.展开更多
Constructing three-dimensional(3D)current collectors has been revealed as an effective strategy to suppress lithium dendrites and extend the lifespan of Li metal batteries.Earlier attempts to improve Li compatibility ...Constructing three-dimensional(3D)current collectors has been revealed as an effective strategy to suppress lithium dendrites and extend the lifespan of Li metal batteries.Earlier attempts to improve Li compatibility have focused on the initial lithium nucleation to increase lithiophilic sites and maximize the electrochemically active areas.However,the subsequent Li growth process and the evolution of the regulation mechanism,which also govern the Li plating behavior,have not beenpreviously exploited in depth.Herein,we report a full-process-adjusted zinc sulfide(ZnS)-rich carbon-based matrix enabling more uniform and oblate Li plating morphology.At the early stage,the in situ formed LiZn alloy offers the lithiophilic region for favorable nucleation and initial deposition while the Li_(2)S component passivates the micro-interface.As plating progresses,the proportion of solid solution(Li_(1−x)Zn_(x))in the conductive substrate gradually increases,replacing LiZn to dominate the deposition morphology.The electrochemical tests confirm the excellent performance of the modified matrix with nano-ZnS decoration,which delivers a high average Coulombic efficiency of about 99%for 100 cycles.Our work furnishes an alternative choice from the sustainable perspective of adjusting Li plating behavior for dendrite-free and long-term Li metal batteries.展开更多
基金finally supported by the National Natural Science Foundation of China(NSFC Grants 52074098)the Major Science and Technology R&D Special Project in Jiangxi Province(104 Ah high specific energy and fast charging function lithium-ion battery system development and application project 20233AAE02009)the Cospowers Technology Co.,Ltd.,Technology Project Funding(research on key materials and battery technologies for sodium ion batteries,KYDY2022003)。
文摘Sodium-ion batteries are promising candidates for next-generation large-scale energy storage owing to their abundance and low cost.Biphasic intercalation reactions,constrained by kinetic limitations and structural instability,fundamentally restrict the rate capability and cycle life of sodium ion batteries.However,precise regulation of these reactions to enhance kinetics remains challenging.Here,we propose a strategy of atomic-scale phase engineering to activate the metastable state and achieve a three-phase reaction through precise Mg^(2+)doping at V sites in Na_(3)V_(2)(PO_(4))_(3).The Mg^(2+)occupancy promotes the exchange between Na1 and Na2 sites,thereby stabilizing a Na_(2)V_(2)(PO_(4))_(3) intermediate.First-principles calculations indicate that Mg^(2+)occupation facilitates charge redistribution by weakening Na-O electrostatic interaction,stabilizing the formation of Na_(2)V_(2)(PO_(4))_(3)phase.The optimized cathode exhibits ultrahigh capacity retention(84.5%after 5000 cycles at 3.51 A g^(-1)),supports ultrafast charging within 120 s,and exceptional rate capability(96.2 mAh g^(-1)at 4.68 A g^(-1)).This work establishes a universal route to unlock hidden reaction pathways by redefining the role of dopants in phase transition control.
基金supported by grants from the National Institutes of Health(SBIR R44 AI125060,NIAMS P50 AR072000,and NIAMS P30 AR069655)。
文摘Eradication of MRSA osteomyelitis requires elimination of distinct biofilms.To overcome this,we developed bisphosphonateconjugated sitafloxacin(BCS,BV600072)and hydroxybisphosphonate-conjugate sitafloxacin(HBCS,BV63072),which achieve“target-and-release”drug delivery proximal to the bone infection and have prophylactic efficacy against MRSA static biofilm in vitro and in vivo.Here we evaluated their therapeutic efficacy in a murine 1-stage exchange femoral plate model with bioluminescent MRSA(USA300LAC::lux).Osteomyelitis was confirmed by CFU on the explants and longitudinal bioluminescent imaging(BLI)after debridement and implant exchange surgery on day 7,and mice were randomized into seven groups:1)Baseline(harvested at day7,no treatment);2)HPBP(bisphosphonate control for BCS)+vancomycin;3)HPHBP(hydroxybisphosphonate control for HBCS)+vancomycin;4)vancomycin;5)sitafloxacin;6)BCS+vancomycin;and 7)HBCS+vancomycin.BLI confirmed infection persisted in all groups except for mice treated with BCS or HBCS+vancomycin.Radiology revealed catastrophic femur fractures in all groups except mice treated with BCS or HBCS+vancomycin,which also displayed decreases in peri-implant bone loss,osteoclast numbers,and biofilm.To confirm this,we assessed the efficacy of vancomycin,sitafloxacin,and HBCS monotherapy in a transtibial implant model.The results showed complete lack of vancomycin efficacy while all mice treated with HBCS had evidence of infection control,and some had evidence of osseous integrated septic implants,suggestive of biofilm eradication.Taken together these studies demonstrate that HBCS adjuvant with standard of care debridement and vancomycin therapy has the potential to eradicate MRSA osteomyelitis.
基金the financial support from Ningbo Science and Technology Bureau(No.2019B10114,the Lithium Battery Step Utilization and Recycling Technology Program of Ningbo).
文摘High capacity Sn_(4)P_(3) is considered as a promising anode candidate for lithium-ion batteries(LIBs),but the fast capacity decay caused by the enormous volume changes and tin agglomeration during cycling largely limits its practical applications.Herein,MWCNTs/Sn_(4)P_(3)@C with a coaxial cable-like structure is designed,where a carbon protective layer is wrapped on the surfaces of Sn_(4)P_(3) nanoparticles to minimize their exposure to the electrolyte and multi-walled carbon nanotubes(MWCNTs)serve as a conductive backbone to disperse Sn_(4)P_(3) nanoparticles.When applied as the lithium container,the MWCNTs/Sn_(4)P_(3)@C composites demonstrate excellent cycling stability(delivering a high reversible capacity of 768.8 mA h g^(-1) after 100 cycles at 100 mA g^(-1) and 569.5 mA h g^(-1) after 1000 cycles at 1000 mA g^(-1))and rate capability(a de-lithiation capacity of 520.1 mA h g^(-1) maintained at a high current density of 2000 mA g^(-1)).Furthermore,full cells composed of the MWCNTs/Sn_(4)P_(3)@C anode and the commercially available LiNi_(1/3)Mn_(1/3)Co_(1/3)O_(2) cathode were also assembled.The result of cycling performance showed a reversible capacity of 507 mA h g^(-1) after 100 cycles,which is far superior to that of bare Sn_(4)P_(3) and MWCNTs/Sn_(4)P_(3) anodes with the reversible capacity lower than 100 mA h g^(-1).These excellent electrochemical performances originate from a synergistic effect between the MWCNT conductive backbone and carbon shell protective layer.The MWCNT backbone can enhance the conductivity and serve as a framework to disperse Sn_(4)P_(3) nanoparticles,thus helping to accommodate the large volume changes during cycling,while the carbon shell not only can further enhance the conductivity but also minimize the side reaction between Sn_(4)P_(3) nanoparticles and electrolytes.
基金supported by the National Natural Science Foundation of China(52074098)the Foundation of Key Program of Sci-Tech Innovation in Ningbo(2019B10114).
文摘Constructing three-dimensional(3D)current collectors has been revealed as an effective strategy to suppress lithium dendrites and extend the lifespan of Li metal batteries.Earlier attempts to improve Li compatibility have focused on the initial lithium nucleation to increase lithiophilic sites and maximize the electrochemically active areas.However,the subsequent Li growth process and the evolution of the regulation mechanism,which also govern the Li plating behavior,have not beenpreviously exploited in depth.Herein,we report a full-process-adjusted zinc sulfide(ZnS)-rich carbon-based matrix enabling more uniform and oblate Li plating morphology.At the early stage,the in situ formed LiZn alloy offers the lithiophilic region for favorable nucleation and initial deposition while the Li_(2)S component passivates the micro-interface.As plating progresses,the proportion of solid solution(Li_(1−x)Zn_(x))in the conductive substrate gradually increases,replacing LiZn to dominate the deposition morphology.The electrochemical tests confirm the excellent performance of the modified matrix with nano-ZnS decoration,which delivers a high average Coulombic efficiency of about 99%for 100 cycles.Our work furnishes an alternative choice from the sustainable perspective of adjusting Li plating behavior for dendrite-free and long-term Li metal batteries.
