MXenes have attracted great interest in various fields,and pillared MXenes open a new path with larger interlayer spacing.However,the further study of pillared MXenes is blocked at multilayered state due to serious re...MXenes have attracted great interest in various fields,and pillared MXenes open a new path with larger interlayer spacing.However,the further study of pillared MXenes is blocked at multilayered state due to serious restacking phenomenon of few-layered MXene nanosheets.In this work,for the first time,we designed a facile NH4+method to fundamentally solve the restacking issues of MXene nanosheets and succeeded in achieving pillared few-layered MXene.Sn nanocomplex pillared few-layered Ti3C2Tx(STCT)composites were synthesized by introducing atomic Sn nanocomplex into interlayer of pillared few-layered Ti3C2Tx MXenes via pillaring technique.The MXene matrix can inhibit Sn nanocomplex particles agglomeration and serve as conductive network.Meanwhile,the Sn nanocomplex particles can further open the interlayer spacing of Ti3C2Tx during lithiation/delithiation processes and therefore generate extra capacity.Benefiting from the“pillar effect,”the STCT composites can maintain 1016 mAh g^?1 after 1200 cycles at 2000 mA g^?1 and deliver a stable capacity of 680 mAh g^?1 at 5 A g^?1,showing one of the best performances among MXene-based composites.This work will provide a new way for the development of pillared MXenes and their energy storage due to significant breakthrough from multilayered state to few-layered one.展开更多
Aqueous rechargeable zinc ion batteries are regarded as a competitive alternative to lithium-ion batteries because of their distinct advantages of high security,high energy density,low cost,and environmental friendlin...Aqueous rechargeable zinc ion batteries are regarded as a competitive alternative to lithium-ion batteries because of their distinct advantages of high security,high energy density,low cost,and environmental friendliness.However,deep-seated problems including Zn dendrite and adverse side reactions severely impede the practical application.In this work,we proposed a freestanding Zn-electrolyte interfacial layer composed of multicapsular carbon fibers(MCFs)to regulate the plating/stripping behavior of Zn anodes.The versatile MCFs protective layer can uniformize the electric field and Zn^(2+)flux,meanwhile,reduce the deposition overpotentials,leading to high-quality and rapid Zn deposition kinetics.Furthermore,the bottom-up and uniform deposition of Zn on the Zn-MCFs interface endows long-term and high-capacity plating.Accordingly,the Zn@MCFs symmetric batteries can keep working up to 1500 h with 5 mAh cm^(−2).The feasibility of the MCFs interfacial layer is also convinced in Zn@MCFs||MnO_(2) batteries.Remarkably,the Zn@MCFs||α-MnO_(2)batteries deliver a high specific capacity of 236.1 mAh g^(−1)at 1 A g^(−1)with excellent stability,and maintain an exhilarating energy density of 154.3 Wh kg^(−1) at 33%depth of discharge in pouch batteries.展开更多
Herein,N-Ti3C2@CNT microspheres are successfully synthesized by the simple spray drying method.In the preparation process,HCl-treated melamine(HTM)is selected as the sources of carbon and nitrogen.It not only realizes...Herein,N-Ti3C2@CNT microspheres are successfully synthesized by the simple spray drying method.In the preparation process,HCl-treated melamine(HTM)is selected as the sources of carbon and nitrogen.It not only realizes in situ growth of CNTs on the surface of MXene nanosheets with the catalysis of Ni,but also introduces efficient N-doping in both MXene and CNTs.Within the microsphere,MXene nanosheets interconnect with CNTs to form porous and conductive network.In addition,N-doped MXene and CNTs can provide strong chemical immobilization for polysulfides and effectively entrap them within the porous microspheres.Above-mentioned merits enable N-Ti3C2@CNT microspheres to be ideal sulfur host.When used in lithium–sulfur(Li–S)battery,the N-Ti3C2@CNT microspheres/S cathode delivers initial specific capacity of 927 mAh g−1 at 1 C and retains high capacity of 775 mAh g−1 after 1000 cycles with extremely low fading rate(FR)of 0.016%per cycle.Furthermore,the cathode still shows high cycling stability at high C-rate of 4 C(capacity of 647 mAh g−1 after 650 cycles,FR 0.027%)and high sulfur loading of 3 and 6 mg cm−2 for Li–S batteries.展开更多
Liver fibrosis is characterized by the excessive accumulation of extracellular matrix(ECM),which is primarily produced by activated hepatic stellate cells(HSCs).However,effective therapies for hepatic fibrosis are cur...Liver fibrosis is characterized by the excessive accumulation of extracellular matrix(ECM),which is primarily produced by activated hepatic stellate cells(HSCs).However,effective therapies for hepatic fibrosis are currently lacking.Artesunate is a promising anti-fibrotic drug candidate,but its clinical application is hindered by limited absorption.Here,we present a novel oral delivery platform that enhances the HSCs uptake of artesunate and induces potent ferroptosis.The platform is vitamin Adecorated nanoparticles encapsulated with artesunate.The multifunctional ligand vitamin A interacts with retinol-binding proteins that are highly expressed on the intestinal epithelium to promote transcytosis,highly expressed on the surface of HSCs but lowly expressed in normal hepatocytes.After oral administration,this oral delivery platform enhances transepithelial transport in the intestine,improves drug accumulation in the liver,and continuously increases HSCs uptake of artesunate.Upon drug release in HSCs,artesunate depletes glutathione peroxidase 4 and glutathione,effectively initiating ferroptosis.In vivo experiments demonstrate that this strategy induces pronounced ferroptosis,efficiently relieving liver fibrosis.This work provides a proof-ofconcept demonstration that an oral delivery strategy for ferroptosis inducers may be beneficial for liver fibrosis treatment.展开更多
Due to easy re-stacking,low yield of few-layered MXenes(f-MXenes),the applications of MXenes are mainly restricted in multi-layered MXenes(m-MXenes)state.Although f-MXenes can be prepared from m-MXenes,after exfoliati...Due to easy re-stacking,low yield of few-layered MXenes(f-MXenes),the applications of MXenes are mainly restricted in multi-layered MXenes(m-MXenes)state.Although f-MXenes can be prepared from m-MXenes,after exfoliation process,a mass of sediments which are still essentially compact MXenes are usually directly discarded,leading to low utilization of raw m-MXenes.Herein,a classified preparation strategy is adopted to exploit the raw m-MXenes and traditional MXenes sediments,taking multi-layered Ti_(3)C_(2)T_(x)MXene as an example.Via rational delamination and subsequent treatment to Ti_(3)C_(2)T_(x)sediments,we succeed in achieving classified and large-scale preparation of various Ti_(3)C_(2)T_(x)MXene derivatives,including few-layered Ti_(3)C_(2)T_(x)(f-Ti_(3)C_(2)T_(x))powders,f-Ti_(3)C_(2)T_(x)films,and Ti_(3)C_(2)T_(x)MXene-derived nanowires with heterostructure of potassium titanate and Ti_(3)C_(2)T_(x).We demonstrate the necessity of“step-by-step delamination”towards traditional Ti_(3)C_(2)T_(x)sediments to improve the yield of f-Ti_(3)C_(2)T_(x)from 15%to 72%;the feasibility of“solution-phase flocculation(SPF)”to fundamentally solve the re-stacking phenomenon,and oxidation degradation issues of f-Ti_(3)C_(2)T_(x)during storage;as well as the convenience of SPF to deal with time-consuming issues of fabricating Ti_(3)C_(2)T_(x)films.What’s more,alkali-heat treatment of final Ti_(3)C_(2)T_(x)sediments turns waste into treasure of Ti_(3)C_(2)T_(x)-derived nanowires,leading to 100%utilization of raw Ti_(3)C_(2)T_(x).The content of one-dimensional(1D)nanowires in the hybrids can be adjusted by controlling alkalization time.The 3D architecture heterostructure composed of 1D nanowires and 2D nanosheets exhibits gorgeous application potential.This work can expand preparation and application of various MXenes derivatives,promoting process of various MXenes.展开更多
Pillaring technologies have been considered as an effective way to improve lithium storage performance of Ti_(3)C_(2)T_(x)MXene.Nevertheless,the pillared hybrids suffer from sluggish Li^(+)diffusion kinetics and elect...Pillaring technologies have been considered as an effective way to improve lithium storage performance of Ti_(3)C_(2)T_(x)MXene.Nevertheless,the pillared hybrids suffer from sluggish Li^(+)diffusion kinetics and electronic transportation due to the compact multi-layered MXene structure,thus exhibiting inferior rate performance.Herein,the few-layered Ti_(3)O_(2)MXene(f-Ti_(3)C_(2)MXene)which is free from restacking can be prepared quickly based on the NH4^(+)ions method.Besides,Fe nanocomplex pillared few-layered Ti_(3)C_(2)T_(x)(FPTC)heterostructures are fabricated via the intercalation of Fe ions into the interlayer of f-Ti_(3)C_(2)MXene.The f-Ti_(3)C_(2)MXene which is immune to restacking can provide a highly conductive substrate for the rapid transport of Li+ions and electrons and possess adequate electrolyte accessible area.Moreover,f-Ti_(3)C_(2)MXene can efficiently relieve the aggregation,prevent the pulverization and buffer the large volume change of Fe nanocomplex during lithiation/delithiation process,leading to enhanced charge transfer kinetics and excellent structural stability of FPTC composites.Consequently,the FPTC hybrids exhibit a high capacity of 535 mAh·g^(-1)after 150 cycles at 0.5 A·g^(-1)and an enhanced rate performance with 310 mAh·g^(-1)after 850 cycles at 5 A·g^(-1).This strategy is facile,universal and can be extended tofabricate various few-layered MXene-derived hybrids with superior rate capability.展开更多
All-solid-state lithium batteries(ASSLBs)employ high-capacity lithium(Li)metal as the anode and exhibit a higher energy density than that of conventional Li-ion batteries.However,the problems arose from the Li dendrit...All-solid-state lithium batteries(ASSLBs)employ high-capacity lithium(Li)metal as the anode and exhibit a higher energy density than that of conventional Li-ion batteries.However,the problems arose from the Li dendrites induce severely parasitic reaction between Li and electrolytes,leading to low coulombic efficiency(CE)and poor cyclic stability.Herein,a poly(vinylidene-co-hexafluoropropylene)/lithium nitrate(PVDF-HFP/LiNO_(3),marked as PFH/LN)artificial layer is employed to modified Li and achieve high CE ASSLBs with polyethylene oxide-Li_(6.4) La_(3)Zr_(1.4)Ta_(0.6)O_(12)(PEO-LLZTO)electrolyte.LN serves as a functionalized additive to facilitate the formation of a robust solid electrolyte interface(SEI),effi-ciently suppressing the formation of Li dendrites.Additionally,LN as a“binder”effectively links PFH with Li,providing good contact.PFH possesses high mechanical strength and moderate flexibility,which can not only physically inhibit the growth of Li dendrites,but also maintain the structural integrity of arti-ficial layer over long-term cycles.Finally,Li/Li cells with such artificial layer demonstrate ultralong cycle life of 1800 and 1000 h under 0.2 and 0.4 mA cm^(-1),respectively.Furtherly,high CE can be achieved when applied in both LiFePO 4 full cells and Li-Cu half cells.This work offers a facile and efficient strategy to greatly promote CE in PEO-based ASSLBs.展开更多
基金the National Natural Science Foundation of China(Grant No.51901206,51822104)the Training Program of Major Basic Research Project of Provincial Natural Science Foundation of Guangdong(2017B030308001).
文摘MXenes have attracted great interest in various fields,and pillared MXenes open a new path with larger interlayer spacing.However,the further study of pillared MXenes is blocked at multilayered state due to serious restacking phenomenon of few-layered MXene nanosheets.In this work,for the first time,we designed a facile NH4+method to fundamentally solve the restacking issues of MXene nanosheets and succeeded in achieving pillared few-layered MXene.Sn nanocomplex pillared few-layered Ti3C2Tx(STCT)composites were synthesized by introducing atomic Sn nanocomplex into interlayer of pillared few-layered Ti3C2Tx MXenes via pillaring technique.The MXene matrix can inhibit Sn nanocomplex particles agglomeration and serve as conductive network.Meanwhile,the Sn nanocomplex particles can further open the interlayer spacing of Ti3C2Tx during lithiation/delithiation processes and therefore generate extra capacity.Benefiting from the“pillar effect,”the STCT composites can maintain 1016 mAh g^?1 after 1200 cycles at 2000 mA g^?1 and deliver a stable capacity of 680 mAh g^?1 at 5 A g^?1,showing one of the best performances among MXene-based composites.This work will provide a new way for the development of pillared MXenes and their energy storage due to significant breakthrough from multilayered state to few-layered one.
基金supported by the National Natural Science Foundation of China(51901206)“the Fundamental Research Funds for the Central Universities”(2021QNA4003).
文摘Aqueous rechargeable zinc ion batteries are regarded as a competitive alternative to lithium-ion batteries because of their distinct advantages of high security,high energy density,low cost,and environmental friendliness.However,deep-seated problems including Zn dendrite and adverse side reactions severely impede the practical application.In this work,we proposed a freestanding Zn-electrolyte interfacial layer composed of multicapsular carbon fibers(MCFs)to regulate the plating/stripping behavior of Zn anodes.The versatile MCFs protective layer can uniformize the electric field and Zn^(2+)flux,meanwhile,reduce the deposition overpotentials,leading to high-quality and rapid Zn deposition kinetics.Furthermore,the bottom-up and uniform deposition of Zn on the Zn-MCFs interface endows long-term and high-capacity plating.Accordingly,the Zn@MCFs symmetric batteries can keep working up to 1500 h with 5 mAh cm^(−2).The feasibility of the MCFs interfacial layer is also convinced in Zn@MCFs||MnO_(2) batteries.Remarkably,the Zn@MCFs||α-MnO_(2)batteries deliver a high specific capacity of 236.1 mAh g^(−1)at 1 A g^(−1)with excellent stability,and maintain an exhilarating energy density of 154.3 Wh kg^(−1) at 33%depth of discharge in pouch batteries.
文摘Herein,N-Ti3C2@CNT microspheres are successfully synthesized by the simple spray drying method.In the preparation process,HCl-treated melamine(HTM)is selected as the sources of carbon and nitrogen.It not only realizes in situ growth of CNTs on the surface of MXene nanosheets with the catalysis of Ni,but also introduces efficient N-doping in both MXene and CNTs.Within the microsphere,MXene nanosheets interconnect with CNTs to form porous and conductive network.In addition,N-doped MXene and CNTs can provide strong chemical immobilization for polysulfides and effectively entrap them within the porous microspheres.Above-mentioned merits enable N-Ti3C2@CNT microspheres to be ideal sulfur host.When used in lithium–sulfur(Li–S)battery,the N-Ti3C2@CNT microspheres/S cathode delivers initial specific capacity of 927 mAh g−1 at 1 C and retains high capacity of 775 mAh g−1 after 1000 cycles with extremely low fading rate(FR)of 0.016%per cycle.Furthermore,the cathode still shows high cycling stability at high C-rate of 4 C(capacity of 647 mAh g−1 after 650 cycles,FR 0.027%)and high sulfur loading of 3 and 6 mg cm−2 for Li–S batteries.
基金supported by the Fundamental Research Funds for the Central Universities(No.SWU-KQ22024)the NMPA Key Laboratory for Research and Evaluation of Pharmaceutical Preparation and Excipients(No.PPE2023005)+3 种基金the China Postdoctoral Science Foundation(No.2023M740731)the Chongqing Science and Technology Commission(No.CSTB2022TIAD-KPX0094)National Key Research and Development Program of China(No.2021YFD1800900)National Natural Science Foundation of China(No.82073790).
文摘Liver fibrosis is characterized by the excessive accumulation of extracellular matrix(ECM),which is primarily produced by activated hepatic stellate cells(HSCs).However,effective therapies for hepatic fibrosis are currently lacking.Artesunate is a promising anti-fibrotic drug candidate,but its clinical application is hindered by limited absorption.Here,we present a novel oral delivery platform that enhances the HSCs uptake of artesunate and induces potent ferroptosis.The platform is vitamin Adecorated nanoparticles encapsulated with artesunate.The multifunctional ligand vitamin A interacts with retinol-binding proteins that are highly expressed on the intestinal epithelium to promote transcytosis,highly expressed on the surface of HSCs but lowly expressed in normal hepatocytes.After oral administration,this oral delivery platform enhances transepithelial transport in the intestine,improves drug accumulation in the liver,and continuously increases HSCs uptake of artesunate.Upon drug release in HSCs,artesunate depletes glutathione peroxidase 4 and glutathione,effectively initiating ferroptosis.In vivo experiments demonstrate that this strategy induces pronounced ferroptosis,efficiently relieving liver fibrosis.This work provides a proof-ofconcept demonstration that an oral delivery strategy for ferroptosis inducers may be beneficial for liver fibrosis treatment.
基金the National Natural ScienceFoundation of China(No.51901206)the fund from Taihu Electric Corporation 0001.
文摘Due to easy re-stacking,low yield of few-layered MXenes(f-MXenes),the applications of MXenes are mainly restricted in multi-layered MXenes(m-MXenes)state.Although f-MXenes can be prepared from m-MXenes,after exfoliation process,a mass of sediments which are still essentially compact MXenes are usually directly discarded,leading to low utilization of raw m-MXenes.Herein,a classified preparation strategy is adopted to exploit the raw m-MXenes and traditional MXenes sediments,taking multi-layered Ti_(3)C_(2)T_(x)MXene as an example.Via rational delamination and subsequent treatment to Ti_(3)C_(2)T_(x)sediments,we succeed in achieving classified and large-scale preparation of various Ti_(3)C_(2)T_(x)MXene derivatives,including few-layered Ti_(3)C_(2)T_(x)(f-Ti_(3)C_(2)T_(x))powders,f-Ti_(3)C_(2)T_(x)films,and Ti_(3)C_(2)T_(x)MXene-derived nanowires with heterostructure of potassium titanate and Ti_(3)C_(2)T_(x).We demonstrate the necessity of“step-by-step delamination”towards traditional Ti_(3)C_(2)T_(x)sediments to improve the yield of f-Ti_(3)C_(2)T_(x)from 15%to 72%;the feasibility of“solution-phase flocculation(SPF)”to fundamentally solve the re-stacking phenomenon,and oxidation degradation issues of f-Ti_(3)C_(2)T_(x)during storage;as well as the convenience of SPF to deal with time-consuming issues of fabricating Ti_(3)C_(2)T_(x)films.What’s more,alkali-heat treatment of final Ti_(3)C_(2)T_(x)sediments turns waste into treasure of Ti_(3)C_(2)T_(x)-derived nanowires,leading to 100%utilization of raw Ti_(3)C_(2)T_(x).The content of one-dimensional(1D)nanowires in the hybrids can be adjusted by controlling alkalization time.The 3D architecture heterostructure composed of 1D nanowires and 2D nanosheets exhibits gorgeous application potential.This work can expand preparation and application of various MXenes derivatives,promoting process of various MXenes.
基金the Tai hu Electric Corporation 0001 and the National Natural Science Foundation o f China(No.51901206).
文摘Pillaring technologies have been considered as an effective way to improve lithium storage performance of Ti_(3)C_(2)T_(x)MXene.Nevertheless,the pillared hybrids suffer from sluggish Li^(+)diffusion kinetics and electronic transportation due to the compact multi-layered MXene structure,thus exhibiting inferior rate performance.Herein,the few-layered Ti_(3)O_(2)MXene(f-Ti_(3)C_(2)MXene)which is free from restacking can be prepared quickly based on the NH4^(+)ions method.Besides,Fe nanocomplex pillared few-layered Ti_(3)C_(2)T_(x)(FPTC)heterostructures are fabricated via the intercalation of Fe ions into the interlayer of f-Ti_(3)C_(2)MXene.The f-Ti_(3)C_(2)MXene which is immune to restacking can provide a highly conductive substrate for the rapid transport of Li+ions and electrons and possess adequate electrolyte accessible area.Moreover,f-Ti_(3)C_(2)MXene can efficiently relieve the aggregation,prevent the pulverization and buffer the large volume change of Fe nanocomplex during lithiation/delithiation process,leading to enhanced charge transfer kinetics and excellent structural stability of FPTC composites.Consequently,the FPTC hybrids exhibit a high capacity of 535 mAh·g^(-1)after 150 cycles at 0.5 A·g^(-1)and an enhanced rate performance with 310 mAh·g^(-1)after 850 cycles at 5 A·g^(-1).This strategy is facile,universal and can be extended tofabricate various few-layered MXene-derived hybrids with superior rate capability.
基金The authors acknowledge the support by Taihu Electric Corpo-ration 0001,the National Natural Science Foundation of China(51901206)the Fundamental Research Funds for the Central Uni-versities(2021QNA4003).
文摘All-solid-state lithium batteries(ASSLBs)employ high-capacity lithium(Li)metal as the anode and exhibit a higher energy density than that of conventional Li-ion batteries.However,the problems arose from the Li dendrites induce severely parasitic reaction between Li and electrolytes,leading to low coulombic efficiency(CE)and poor cyclic stability.Herein,a poly(vinylidene-co-hexafluoropropylene)/lithium nitrate(PVDF-HFP/LiNO_(3),marked as PFH/LN)artificial layer is employed to modified Li and achieve high CE ASSLBs with polyethylene oxide-Li_(6.4) La_(3)Zr_(1.4)Ta_(0.6)O_(12)(PEO-LLZTO)electrolyte.LN serves as a functionalized additive to facilitate the formation of a robust solid electrolyte interface(SEI),effi-ciently suppressing the formation of Li dendrites.Additionally,LN as a“binder”effectively links PFH with Li,providing good contact.PFH possesses high mechanical strength and moderate flexibility,which can not only physically inhibit the growth of Li dendrites,but also maintain the structural integrity of arti-ficial layer over long-term cycles.Finally,Li/Li cells with such artificial layer demonstrate ultralong cycle life of 1800 and 1000 h under 0.2 and 0.4 mA cm^(-1),respectively.Furtherly,high CE can be achieved when applied in both LiFePO 4 full cells and Li-Cu half cells.This work offers a facile and efficient strategy to greatly promote CE in PEO-based ASSLBs.
