Lead halide perovskite(LHP)nanocrystals(NCs)suffer from poor stability against environmental factors(heat,moisture,oxygen,etc.),which seriously hinders their practical application.Constructing a core-shell structure c...Lead halide perovskite(LHP)nanocrystals(NCs)suffer from poor stability against environmental factors(heat,moisture,oxygen,etc.),which seriously hinders their practical application.Constructing a core-shell structure could be an effective approach to improve the stability and optical properties of the LHP NCs.Herein,a novel strategy of water-triggered phase transformation and phospholipid(DSPE)micelle encapsulation is proposed,generating highly luminescent water-dispersed CsPbBr_(3)@CsPb_(2)Br5@DSPE core-shell-shell nanocrystals.The epitaxial growth of the CsPb_(2)Br5 shell is induced by the in-situ reconstruc-tion of the CsPbBr_(3) surface by water erosion,and the lattice mismatch with the CsPbBr_(3) core is small(3.8%).The further amphipathic phospholipid encapsulation guarantees their excellent water dispersity and stability.Revealed by the femtosecond transient absorption spectroscopy,the dense CsPb_(2)Br5@DSPE shell effectively passivates the surface of the CsPbBr_(3) core,thus improving its stability and luminescence performance.The resulting CsPbBr_(3)@CsPb_(2)Br5@DSPE nanoparticles exhibit excellent performance as fluo-rescent probes for bioimaging,aqueous inks for high-resolution pattering,and light conversion layers for LEDs,demonstrating their promising potential in multiple applications.展开更多
Two-dimensional(2D)covalent organic framework nanosheets(CONs)are attracting increasing research attention because of their unique properties derived from their ultrathin thickness,high surface-tovolume atomic ratio,a...Two-dimensional(2D)covalent organic framework nanosheets(CONs)are attracting increasing research attention because of their unique properties derived from their ultrathin thickness,high surface-tovolume atomic ratio,and extremely large surface area.2D CONs can provide high transport pathways for charge carriers(e.g.,electrons,holes and ions)through either the conjugated skeletons or the open channels.Therefore,they have shown great potential in energy related applications.In this review,we firstly introduce the recent developments and characteristics of 2D CONs by focusing on the two typical synthetic methods,i.e.,top-down and bottom-up methods.Then,the energy-related applications in energy storage and conversion of 2D CONs are summarized.Finally,we give our personal views on the challenges and perspectives for the future research of 2D CONs and their composites.展开更多
The doping process and thermoelectric properties of donor-acceptor(D-A)type copolymers are investigated with the representative poly([2,6-4,8-di(5-ethylhexylthienyl)benzo[1,2-b;3,3-b]dithiophene]3-fluoro-2-[(2-ethylhe...The doping process and thermoelectric properties of donor-acceptor(D-A)type copolymers are investigated with the representative poly([2,6-4,8-di(5-ethylhexylthienyl)benzo[1,2-b;3,3-b]dithiophene]3-fluoro-2-[(2-ethylhexyl)-carbonyl]thieno[3,4-b]thiophenediyl))(PTB7-Th).The PTB7-Th is doped by Fe Cl;and only polarons are induced in its doped films.The results reveal that the electron-rich donor units within PTB7-Th lose electrons preferentially at the initial stage of the oxidation and then the acceptor units begin to be oxidized at a high doping concentration.The energy levels of polarons and the Fermi level of the doped PTB7-Th remain almost unchange with different doping levels.However,the morphology of the PTB7-Th films could be deteriorated as the doping levels are improved,which is one of the main reasons for the decrease of electrical conductivity at the later stage of doping.The best electrical conductivity and power factor are obtained to be 42.3 S·cm^(-1);and 33.9μW·mK^(-1),respectively,in the doped PTB7-Th film at room temperature.The power factor is further improved to 38.3μW·mK^(-1);at 75℃.This work may provide meaningful experience for development of D-A type thermoelectric copolymers and may further improve the doping efficiency.展开更多
The exploration of low-cost and metal-free nanozymes with oxidase-mimicking activity is highly desired due to their attractive properties and potential applications.However,it is still challenging and remains unexploi...The exploration of low-cost and metal-free nanozymes with oxidase-mimicking activity is highly desired due to their attractive properties and potential applications.However,it is still challenging and remains unexploited to fully realize oxidase-like nanozyme in the emerging covalent organic frameworks(COFs)due to their polymeric nature and weak photoelectric activity.We herein report the first example of the preparation and oxidase-mimicking activity of novel ultrathin two-dimensional(2D)COF(termed as TTPA-COF)nanosheets.The ultrathin TTPA-COF nanosheets with hexagonal layered structure are constructed from two flexible photoactive(diarylamino)benzene-based linkers,and exhibit remarkable catalytic activity toward the oxidation of 3,3',5,5'-tetramethylbenzidine(TMB)in the presence of O_(2) due to their large specific surface areas and abundant active sites.Moreover,it is worth noting that the nanozyme activity could be regulated by external light irradiation.Based on the oxidasemimicking activity of TTPA-COF nanosheets,a green colorimetric sensor is proposed for the sensitive and selective determination of glutathione(GSH)in a wide linear range of 0.5–40μM with a detection limit of 0.5μM.This work reported here would open new avenues for the exploration of low-cost and high-efficiency nanozymes,as well as extend the application of 2D COF nanosheets in the fields of catalysis and sensing.展开更多
We collected blood from coronavirus disease 2019(COVID-19)convalescent individuals and investigated SARS-CoV-2-specific humoral and cellular immunity in these discharged patients.Follow-up analysis in a cohort of 171 ...We collected blood from coronavirus disease 2019(COVID-19)convalescent individuals and investigated SARS-CoV-2-specific humoral and cellular immunity in these discharged patients.Follow-up analysis in a cohort of 171 patients at 4-11 months after the onset revealed high levels of IgG antibodies.A total of 78.1%(164/210)of the specimens tested positive for neutralizing antibody(NAb).SARS-CoV-2 antigen peptide pools-stimulated-IL-2 and-IFN-y response can distinguish COVID-19 convalescent individuals from healthy donors.Interestingly,NAb survival was significantly affected by the antigen peptide pools-stimulated-IL-2 response,-IL-8 response,and-IFN-y response.The antigen peptide pools-activated CD8+T cell counts were correlated with NAb.The antigen peptide pools-activated natural killer(NK)cell counts in convalescent individuals were correlated with NAb and disease severity.Our data suggested that the development of NAb is associated with the activation of T cells and NK cells.Our work provides a basis for further analysis of the protective immunity to SARS-CoV-2 and for understanding the pathogenesis of COVID-19.It also has implications for the development of an effective vaccine for SARS-CoV-2 infection.展开更多
The exploration of bifunctional electrocatalysts with high catalytic activity and long-term durability for low-temperature Zn-air batteries(ZABs)is an ongoing challenge.Here,quintet-shelled hollow spheres,P-doped mult...The exploration of bifunctional electrocatalysts with high catalytic activity and long-term durability for low-temperature Zn-air batteries(ZABs)is an ongoing challenge.Here,quintet-shelled hollow spheres,P-doped multi-layer Co_(3)O_(4)(PM-Co_(3)O_(4)),with enriched oxygen vacancies are prepared by thermally induced mass relocation and a simple phosphating process.Various advanced characterizations reveal P anion-induced effects on internal electronic structure and local coordination environment.The finite element method elucidates that the complex multi-layer spherical nanostructure is conducive to the transport and diffusion of OH-and O_(2).Benefiting from its unique structural features and abundant oxygen vacancies,the well-designed PM-Co_(3)O_(4) presents small reversible oxygen overpotential for catalyzing oxygen reduction/evolution reactions.Accordingly,the fabricated low-temperature ZABs based on PM-Co_(3)O_(4) as air-cathode exhibit high power density(20.8 mW·cm^(-2))and long-term stability(over 600 cycles)at the ultra-low temperature of-40℃,outperforming state-of-art Pt/C+IrO_(2)-based ZABs.Furthermore,the dynamic evolution mechanism of cobalt oxide catalysts during ZAB operation is elucidated.This work provides a guideline to design efficient electrocatalysts with regulated electronic configurations and exquisite nano-/microstructures for ZABs under extreme working conditions.展开更多
After online publication of the article1 the authors noticed an error in the figure legends of Fig.1 and Supplementary Materials Fig.S2,where the"*P<0.05,0.05<**P<0.001,***P<0.001W.should be replaced ...After online publication of the article1 the authors noticed an error in the figure legends of Fig.1 and Supplementary Materials Fig.S2,where the"*P<0.05,0.05<**P<0.001,***P<0.001W.should be replaced by n*P<0.05,**P<0.01,***P<0.001M.The original article has been corrected.展开更多
基金support from the National Natural Science Foundation of China(Nos.U1905213 and 52303132)the Natural Science Foundation of Hubei Province(No.2024AFB142)the Scientific Research Fund Project of Wuhan Institute of Technology(No.K2023109).
文摘Lead halide perovskite(LHP)nanocrystals(NCs)suffer from poor stability against environmental factors(heat,moisture,oxygen,etc.),which seriously hinders their practical application.Constructing a core-shell structure could be an effective approach to improve the stability and optical properties of the LHP NCs.Herein,a novel strategy of water-triggered phase transformation and phospholipid(DSPE)micelle encapsulation is proposed,generating highly luminescent water-dispersed CsPbBr_(3)@CsPb_(2)Br5@DSPE core-shell-shell nanocrystals.The epitaxial growth of the CsPb_(2)Br5 shell is induced by the in-situ reconstruc-tion of the CsPbBr_(3) surface by water erosion,and the lattice mismatch with the CsPbBr_(3) core is small(3.8%).The further amphipathic phospholipid encapsulation guarantees their excellent water dispersity and stability.Revealed by the femtosecond transient absorption spectroscopy,the dense CsPb_(2)Br5@DSPE shell effectively passivates the surface of the CsPbBr_(3) core,thus improving its stability and luminescence performance.The resulting CsPbBr_(3)@CsPb_(2)Br5@DSPE nanoparticles exhibit excellent performance as fluo-rescent probes for bioimaging,aqueous inks for high-resolution pattering,and light conversion layers for LEDs,demonstrating their promising potential in multiple applications.
基金the Class D of Qianjiang Talent Program(No.ZD20011250001)the start-up grant(No.2019125016829)in Zhejiang University of Technology+1 种基金the financial support from the funding of"Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang"(No.2020R01002)the financial support from the National Natural Science Foundation of China(No.51907173)。
文摘Two-dimensional(2D)covalent organic framework nanosheets(CONs)are attracting increasing research attention because of their unique properties derived from their ultrathin thickness,high surface-tovolume atomic ratio,and extremely large surface area.2D CONs can provide high transport pathways for charge carriers(e.g.,electrons,holes and ions)through either the conjugated skeletons or the open channels.Therefore,they have shown great potential in energy related applications.In this review,we firstly introduce the recent developments and characteristics of 2D CONs by focusing on the two typical synthetic methods,i.e.,top-down and bottom-up methods.Then,the energy-related applications in energy storage and conversion of 2D CONs are summarized.Finally,we give our personal views on the challenges and perspectives for the future research of 2D CONs and their composites.
基金supported by the National Key Research and Development Program of China(Grant No.Q2019YFE0107200)。
文摘The doping process and thermoelectric properties of donor-acceptor(D-A)type copolymers are investigated with the representative poly([2,6-4,8-di(5-ethylhexylthienyl)benzo[1,2-b;3,3-b]dithiophene]3-fluoro-2-[(2-ethylhexyl)-carbonyl]thieno[3,4-b]thiophenediyl))(PTB7-Th).The PTB7-Th is doped by Fe Cl;and only polarons are induced in its doped films.The results reveal that the electron-rich donor units within PTB7-Th lose electrons preferentially at the initial stage of the oxidation and then the acceptor units begin to be oxidized at a high doping concentration.The energy levels of polarons and the Fermi level of the doped PTB7-Th remain almost unchange with different doping levels.However,the morphology of the PTB7-Th films could be deteriorated as the doping levels are improved,which is one of the main reasons for the decrease of electrical conductivity at the later stage of doping.The best electrical conductivity and power factor are obtained to be 42.3 S·cm^(-1);and 33.9μW·mK^(-1),respectively,in the doped PTB7-Th film at room temperature.The power factor is further improved to 38.3μW·mK^(-1);at 75℃.This work may provide meaningful experience for development of D-A type thermoelectric copolymers and may further improve the doping efficiency.
基金supported by the financial support from the National Natural Science Foundation of China(NSFC)(Nos.21976166,22006122,and 21405144)the research funding of“Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang”(No.2020R01002)+4 种基金the Class D of Qianjiang Talent Program(No.ZD20011250001)the Science Challenge Project(No.TZ2016004)he Project of State Key Laboratory of Environment-friendly Energy Materials(No.18zd320303)the Scientific Research Starting Foundation for Returned Overseas Chinese Scholars of Sichuan Province(No.19zd3200)support from the Opening Project of Jiangsu Province Engineering Research Center of Agricultural Breeding Pollution Control and Resource(No.2021ABPCR004).
文摘The exploration of low-cost and metal-free nanozymes with oxidase-mimicking activity is highly desired due to their attractive properties and potential applications.However,it is still challenging and remains unexploited to fully realize oxidase-like nanozyme in the emerging covalent organic frameworks(COFs)due to their polymeric nature and weak photoelectric activity.We herein report the first example of the preparation and oxidase-mimicking activity of novel ultrathin two-dimensional(2D)COF(termed as TTPA-COF)nanosheets.The ultrathin TTPA-COF nanosheets with hexagonal layered structure are constructed from two flexible photoactive(diarylamino)benzene-based linkers,and exhibit remarkable catalytic activity toward the oxidation of 3,3',5,5'-tetramethylbenzidine(TMB)in the presence of O_(2) due to their large specific surface areas and abundant active sites.Moreover,it is worth noting that the nanozyme activity could be regulated by external light irradiation.Based on the oxidasemimicking activity of TTPA-COF nanosheets,a green colorimetric sensor is proposed for the sensitive and selective determination of glutathione(GSH)in a wide linear range of 0.5–40μM with a detection limit of 0.5μM.This work reported here would open new avenues for the exploration of low-cost and high-efficiency nanozymes,as well as extend the application of 2D COF nanosheets in the fields of catalysis and sensing.
基金This work was supported by the National Key Research and Development Program of China(2018YFE0204500)Centrally Guided Hubei Provincial Science and Technology Development Fund Project(2020ZYYD012)the Key Project for Anti-2019 Novel Coronavirus Pneumonia from the National Key Research and Development Program of China(2020YFC0845500).
文摘We collected blood from coronavirus disease 2019(COVID-19)convalescent individuals and investigated SARS-CoV-2-specific humoral and cellular immunity in these discharged patients.Follow-up analysis in a cohort of 171 patients at 4-11 months after the onset revealed high levels of IgG antibodies.A total of 78.1%(164/210)of the specimens tested positive for neutralizing antibody(NAb).SARS-CoV-2 antigen peptide pools-stimulated-IL-2 and-IFN-y response can distinguish COVID-19 convalescent individuals from healthy donors.Interestingly,NAb survival was significantly affected by the antigen peptide pools-stimulated-IL-2 response,-IL-8 response,and-IFN-y response.The antigen peptide pools-activated CD8+T cell counts were correlated with NAb.The antigen peptide pools-activated natural killer(NK)cell counts in convalescent individuals were correlated with NAb and disease severity.Our data suggested that the development of NAb is associated with the activation of T cells and NK cells.Our work provides a basis for further analysis of the protective immunity to SARS-CoV-2 and for understanding the pathogenesis of COVID-19.It also has implications for the development of an effective vaccine for SARS-CoV-2 infection.
基金supported by the Natural Science Foundation of Guangdong Province(Nos.2021A1515010504,2022A1515010049)the National Natural Science Foundation of China(Nos.21706090,52172202,51872124)+1 种基金the Major Technological Innovation Project of Hubei Science and Technology Department(No.2019AAA164)the Natural Science Foundation of Guangzhou(No.201904010049).
文摘The exploration of bifunctional electrocatalysts with high catalytic activity and long-term durability for low-temperature Zn-air batteries(ZABs)is an ongoing challenge.Here,quintet-shelled hollow spheres,P-doped multi-layer Co_(3)O_(4)(PM-Co_(3)O_(4)),with enriched oxygen vacancies are prepared by thermally induced mass relocation and a simple phosphating process.Various advanced characterizations reveal P anion-induced effects on internal electronic structure and local coordination environment.The finite element method elucidates that the complex multi-layer spherical nanostructure is conducive to the transport and diffusion of OH-and O_(2).Benefiting from its unique structural features and abundant oxygen vacancies,the well-designed PM-Co_(3)O_(4) presents small reversible oxygen overpotential for catalyzing oxygen reduction/evolution reactions.Accordingly,the fabricated low-temperature ZABs based on PM-Co_(3)O_(4) as air-cathode exhibit high power density(20.8 mW·cm^(-2))and long-term stability(over 600 cycles)at the ultra-low temperature of-40℃,outperforming state-of-art Pt/C+IrO_(2)-based ZABs.Furthermore,the dynamic evolution mechanism of cobalt oxide catalysts during ZAB operation is elucidated.This work provides a guideline to design efficient electrocatalysts with regulated electronic configurations and exquisite nano-/microstructures for ZABs under extreme working conditions.
文摘After online publication of the article1 the authors noticed an error in the figure legends of Fig.1 and Supplementary Materials Fig.S2,where the"*P<0.05,0.05<**P<0.001,***P<0.001W.should be replaced by n*P<0.05,**P<0.01,***P<0.001M.The original article has been corrected.
