As promising energy storage systems,lithium-sulfur(Li-S)batteries have attracted significant attention because of their ultra-high energy densities.However,Li-S battery suffers problems related to the complex phase co...As promising energy storage systems,lithium-sulfur(Li-S)batteries have attracted significant attention because of their ultra-high energy densities.However,Li-S battery suffers problems related to the complex phase conversion that occurs during the charge-discharge process,particularly the deposition of solid Li2S from the liquid-phase polysulfides,which greatly limits its practical application.In this paper,edge-rich MoS2/C hollow microspheres(Edg-MoS2/C HMs)were designed and used to functionalize separator for Li-S battery,resulting in the uniform deposition of Li2S.The microspheres were fabricated through the facile hydrothermal treatment of MoO3-aniline nanowires and a subsequent carbonization process.The obtained Edg-MoS2/C HMs have a strong chemical absorption capability and high density of Li2S binding sites,and exhibit excellent electrocatalytic performance and can effectively hinder the polysulfide shuttle effect and guide the uniform nucleation and growth of Li2S.Furthermore,we demonstrate that the Edg-MoS2/C HMs can effectively regulate the deposition of Li2S and significantly improve the reversibility of the phase conversion of the active sulfur species,especially at high sulfur loadings and high C-rates.As a result,a cell containing a separator functionalized with Edg-MoS2/C HMs exhibited an initial discharge capacity of 935 mAh g-1 at 1.0 C and maintained a capacity of 494 mAh g-1 after 1000 cycles with a sulfur loading of 1.7 mg cm-2.Impressively,at a high sulfur loading of 6.1 mg cm-2 and high rate of 0.5 C,the cell still delivered a high reversible discharge capacity of 478 mAh g-1 after 300 cycles.This work provides fresh insights into energy storage systems related to complex phase conversions.展开更多
The low sulfur utilization and fast capacity fading resulting from the sluggish redox reaction and abominable polysulfides shuttle greatly hinder the practical applications of lithium-sulfur(Li-S) batteries.Herein, we...The low sulfur utilization and fast capacity fading resulting from the sluggish redox reaction and abominable polysulfides shuttle greatly hinder the practical applications of lithium-sulfur(Li-S) batteries.Herein, we develop a facile "in-situ growth" method to decorate ultra-small Mo2 C nanoparticles(USMo2 C) on the surface of Ketjen Black(KB) to functionalize the commercial polypropylene(PP) separators,which can accelerate the redox kinetics of lithium polysulfides conversion and effectively increase the utilization of sulfur for Li-S batteries. Importantly, the US-Mo2 C nanoparticles have abundant sites for chemical adsorption towards polysulfides and the conductive carbon networks of KB have cross-linked pore channels, which can promote electron transport and provide physical barrier and volume expansion space for polysulfides. Due to the combined effects of the US-Mo2 C and KB, Li-S cells employing the multifunctional PP separators modified with KB/US-Mo2 C composite(KB/US-Mo2 C@PP) exhibit a high specific capacity(1212.8 mAh g^(-1) at 0.2 C), and maintain a reversible capacity of 1053.3 m Ah g^(-1) after 100 cycles.More importantly, the KB/US-Mo2 C@PP cells with higher sulfur mass loading of 4.9 mg cm^(-2) have superb areal capacity of 2.3 mAh cm^(-2). This work offers a novel and promising perspective for high-performance Li-S batteries from both the shuttle effect and the complex polysulfides conversion.展开更多
Organic long-persistent luminescence(LPL)materials,featuring low preparation cost,eco-friendly synthesis,and easy modification of functional groups,have exhibited extensive applications in information encryption,anti-...Organic long-persistent luminescence(LPL)materials,featuring low preparation cost,eco-friendly synthesis,and easy modification of functional groups,have exhibited extensive applications in information encryption,anti-counterfeiting,and biological imaging.Several design strategies including crystallization-inducement,H-aggregation,and host-guest doping to enhance persistent-room-temperature phosphorescence(RTP)effect by precisely controlling intersystem crossing(ISC)constant and suppressing nonradiative decay rates,those are important strategies to enable LPL performance.Among the strategies,researchers have made several efforts to enhance persistent-RTP effect by host-guest interaction,in which the host matrices provide a rigid environment for phosphor guest molecules.The interaction of the luminescent guest molecules with the host matrix can effectively reduce the vibration and rotation of the luminescent molecules,and suppress the non-radiative inactivation,thereby improving the phosphorescence quantum yield.This review aims to summarize several design strategies of pure organic LPL materials based on persistent-RTP effect through host-guest interaction,and describe some applications of pure organic LPL materials in different fields.展开更多
Arterial vasospasm after microsurgery can cause severe obstruction of blood flow manifested as low tissue temperature,leading to tissue necrosis.The timely discovery and synchronized treatment become pivotal.In this s...Arterial vasospasm after microsurgery can cause severe obstruction of blood flow manifested as low tissue temperature,leading to tissue necrosis.The timely discovery and synchronized treatment become pivotal.In this study,a reversible,intelligent,responsive thermosensitive hydrogel system is constructed employing both the gel–sol transition and the sol–gel transition.The“reversible thermosensitive(RTS)”hydrogel loaded with verapamil hydrochloride is designed to dynamically and continuously regulate the extravascular microenvi-ronment by inhibiting extracellular calcium influx.After accurate implantation and following in situ gelation,the RTS hydrogel reverses to the sol state causing massive drug release to inhibit vasospasm when the tissue tem-perature drops to the predetermined transition temperature.Subsequent restoration of the blood supply allevi-ates further tissue injury.Before the temperature drops,the RTS hydrogel maintains the gel state as a sustained-release reservoir to prevent vasospasm.The inhibition of calcium influx and vasospasm in vitro and in vivo is demonstrated using vascular smooth muscle cells,mice mesenteric arterial rings,and vascular ultrasonic Doppler detection.Subsequent animal experiments demonstrate that RTS hydrogel can promote tissue survival and alleviate tissue injury responding to temperature change.Therefore,this RTS hydrogel holds therapeutic po-tential for diseases requiring timely detection of temperature change.展开更多
锂硫电池固有的缓慢转化动力学和严重的穿梭效应导致其可逆容量和循环寿命差,严重阻碍了其实际应用.为了解决这些问题,我们设计并构建了一种Ni/Ni_(2)P异质结嵌入介孔碳纳米球的复合材料(Ni/Ni_(2)P-MCN),将其用于锂硫电池隔膜改性以促...锂硫电池固有的缓慢转化动力学和严重的穿梭效应导致其可逆容量和循环寿命差,严重阻碍了其实际应用.为了解决这些问题,我们设计并构建了一种Ni/Ni_(2)P异质结嵌入介孔碳纳米球的复合材料(Ni/Ni_(2)P-MCN),将其用于锂硫电池隔膜改性以促进多硫化物的催化转化.研究发现,Ni/Ni_(2)P-MCN改性隔膜可以通过丰富的异质结化学吸附位点吸附多硫化物、抑制穿梭效应,而且对多硫化物的转化具有优异的催化活性.此外,具有暴露介孔结构的导电碳球可以作为物理屏障,容纳沉积的不溶性Li_(2)S.因此,使用Ni/Ni_(2)P-MCN改性隔膜的电池显示出优异的倍率性能(5 C下431 mA h g^(-1))和循环稳定性(1500次循环下平均容量衰减约0.031%).在4.2 mg cm^(-2)的高载硫下,输出面积比容量约3.5 mA h cm^(-2).我们认为,这种独特的Ni/Ni_(2)P异质结/多孔碳复合材料在高性能、可持续储能器件中具备巨大的应用潜力.展开更多
基金financially supported by National Natural Science Foundation of China (No. 51672083)Program of Shanghai Academic/Technology Research Leader (18XD1401400)+3 种基金Basic Research Program of Shanghai (17JC1404702)Leading talents in Shanghai in 2018The 111 project (B14018)the Fundamental Research Funds for the Central Universities (222201718002)
文摘As promising energy storage systems,lithium-sulfur(Li-S)batteries have attracted significant attention because of their ultra-high energy densities.However,Li-S battery suffers problems related to the complex phase conversion that occurs during the charge-discharge process,particularly the deposition of solid Li2S from the liquid-phase polysulfides,which greatly limits its practical application.In this paper,edge-rich MoS2/C hollow microspheres(Edg-MoS2/C HMs)were designed and used to functionalize separator for Li-S battery,resulting in the uniform deposition of Li2S.The microspheres were fabricated through the facile hydrothermal treatment of MoO3-aniline nanowires and a subsequent carbonization process.The obtained Edg-MoS2/C HMs have a strong chemical absorption capability and high density of Li2S binding sites,and exhibit excellent electrocatalytic performance and can effectively hinder the polysulfide shuttle effect and guide the uniform nucleation and growth of Li2S.Furthermore,we demonstrate that the Edg-MoS2/C HMs can effectively regulate the deposition of Li2S and significantly improve the reversibility of the phase conversion of the active sulfur species,especially at high sulfur loadings and high C-rates.As a result,a cell containing a separator functionalized with Edg-MoS2/C HMs exhibited an initial discharge capacity of 935 mAh g-1 at 1.0 C and maintained a capacity of 494 mAh g-1 after 1000 cycles with a sulfur loading of 1.7 mg cm-2.Impressively,at a high sulfur loading of 6.1 mg cm-2 and high rate of 0.5 C,the cell still delivered a high reversible discharge capacity of 478 mAh g-1 after 300 cycles.This work provides fresh insights into energy storage systems related to complex phase conversions.
基金financially supported by the National Natural Science Foundation of China for Innovative Research Groups (No. 51621002)the National Key Research and Development Program of China (Grant No. 2016YFA0203700)+5 种基金NSFC (Grant No 51672083)Program of Shanghai Academic/Technology Research Leader (18XD1401400)Basic Research Program of Shanghai (17JC1404702)Leading talents in Shanghai in 2018The Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning, the 111 project (B14018)The Fundamental Research Funds for Central Universities (222201718002)。
文摘The low sulfur utilization and fast capacity fading resulting from the sluggish redox reaction and abominable polysulfides shuttle greatly hinder the practical applications of lithium-sulfur(Li-S) batteries.Herein, we develop a facile "in-situ growth" method to decorate ultra-small Mo2 C nanoparticles(USMo2 C) on the surface of Ketjen Black(KB) to functionalize the commercial polypropylene(PP) separators,which can accelerate the redox kinetics of lithium polysulfides conversion and effectively increase the utilization of sulfur for Li-S batteries. Importantly, the US-Mo2 C nanoparticles have abundant sites for chemical adsorption towards polysulfides and the conductive carbon networks of KB have cross-linked pore channels, which can promote electron transport and provide physical barrier and volume expansion space for polysulfides. Due to the combined effects of the US-Mo2 C and KB, Li-S cells employing the multifunctional PP separators modified with KB/US-Mo2 C composite(KB/US-Mo2 C@PP) exhibit a high specific capacity(1212.8 mAh g^(-1) at 0.2 C), and maintain a reversible capacity of 1053.3 m Ah g^(-1) after 100 cycles.More importantly, the KB/US-Mo2 C@PP cells with higher sulfur mass loading of 4.9 mg cm^(-2) have superb areal capacity of 2.3 mAh cm^(-2). This work offers a novel and promising perspective for high-performance Li-S batteries from both the shuttle effect and the complex polysulfides conversion.
基金o National Natural Science Foundation of China(No.22178263)Natural Science Foundation of Tianjin City(No.22JCQNJC00770)Haihe Laboratory of Sustainable Chemical Transformations.The authors also thank Mr.Ben Parks from the Southern Illinois University Carbondale for proofreading the manuscript.
文摘Organic long-persistent luminescence(LPL)materials,featuring low preparation cost,eco-friendly synthesis,and easy modification of functional groups,have exhibited extensive applications in information encryption,anti-counterfeiting,and biological imaging.Several design strategies including crystallization-inducement,H-aggregation,and host-guest doping to enhance persistent-room-temperature phosphorescence(RTP)effect by precisely controlling intersystem crossing(ISC)constant and suppressing nonradiative decay rates,those are important strategies to enable LPL performance.Among the strategies,researchers have made several efforts to enhance persistent-RTP effect by host-guest interaction,in which the host matrices provide a rigid environment for phosphor guest molecules.The interaction of the luminescent guest molecules with the host matrix can effectively reduce the vibration and rotation of the luminescent molecules,and suppress the non-radiative inactivation,thereby improving the phosphorescence quantum yield.This review aims to summarize several design strategies of pure organic LPL materials based on persistent-RTP effect through host-guest interaction,and describe some applications of pure organic LPL materials in different fields.
基金National Key Research and Development Program of China(2020YFA0908200)National Natural Science Foundation of China(81772099,81801928 and 52103173)+3 种基金China Postdoctoral Science Foundation(2021M692105)Shanghai Municipal Health Commission(20204Y0354)Shanghai Municipal Key Clinical Specialty(shslczdzk00901)Young Physicians Innovation Team Project of the Ninth People’s Hospital of Shanghai Jiao Tong University School of Medicine(QC201902).
文摘Arterial vasospasm after microsurgery can cause severe obstruction of blood flow manifested as low tissue temperature,leading to tissue necrosis.The timely discovery and synchronized treatment become pivotal.In this study,a reversible,intelligent,responsive thermosensitive hydrogel system is constructed employing both the gel–sol transition and the sol–gel transition.The“reversible thermosensitive(RTS)”hydrogel loaded with verapamil hydrochloride is designed to dynamically and continuously regulate the extravascular microenvi-ronment by inhibiting extracellular calcium influx.After accurate implantation and following in situ gelation,the RTS hydrogel reverses to the sol state causing massive drug release to inhibit vasospasm when the tissue tem-perature drops to the predetermined transition temperature.Subsequent restoration of the blood supply allevi-ates further tissue injury.Before the temperature drops,the RTS hydrogel maintains the gel state as a sustained-release reservoir to prevent vasospasm.The inhibition of calcium influx and vasospasm in vitro and in vivo is demonstrated using vascular smooth muscle cells,mice mesenteric arterial rings,and vascular ultrasonic Doppler detection.Subsequent animal experiments demonstrate that RTS hydrogel can promote tissue survival and alleviate tissue injury responding to temperature change.Therefore,this RTS hydrogel holds therapeutic po-tential for diseases requiring timely detection of temperature change.
基金supported by the National Key Research and Development Program of China(2020YFA0908200)the National Natural Science Foundation of China(82272263,82002053,and 82202467)+2 种基金Shanghai Municipal Health Commission(20204Y0354)Shanghai Science and Technology Development Funds(22YF1421400)Shanghai Clinical Research Center of Plastic and Reconstructive Surgery supported by Science and Technology Commission of Shanghai Municipality(22MC1940300)。
基金financially supported by the National Natural Science Foundation of China(52072124)Shanghai Municipal Science and Technology Major Project(2018SHZDZX03)+3 种基金the Natural Science Foundation of Shanghai(20ZR1414900)the Leading Talents in Shanghai in2018the Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learningthe 111 Project(B14018)。
文摘锂硫电池固有的缓慢转化动力学和严重的穿梭效应导致其可逆容量和循环寿命差,严重阻碍了其实际应用.为了解决这些问题,我们设计并构建了一种Ni/Ni_(2)P异质结嵌入介孔碳纳米球的复合材料(Ni/Ni_(2)P-MCN),将其用于锂硫电池隔膜改性以促进多硫化物的催化转化.研究发现,Ni/Ni_(2)P-MCN改性隔膜可以通过丰富的异质结化学吸附位点吸附多硫化物、抑制穿梭效应,而且对多硫化物的转化具有优异的催化活性.此外,具有暴露介孔结构的导电碳球可以作为物理屏障,容纳沉积的不溶性Li_(2)S.因此,使用Ni/Ni_(2)P-MCN改性隔膜的电池显示出优异的倍率性能(5 C下431 mA h g^(-1))和循环稳定性(1500次循环下平均容量衰减约0.031%).在4.2 mg cm^(-2)的高载硫下,输出面积比容量约3.5 mA h cm^(-2).我们认为,这种独特的Ni/Ni_(2)P异质结/多孔碳复合材料在高性能、可持续储能器件中具备巨大的应用潜力.