The effective detection of trace methyl mercaptan(CH_(3)SH)with low power consumption is crucial for assessing air quality and facilitating non-invasive diagnosis of diseases such as periodontitis.Herein,we synthesize...The effective detection of trace methyl mercaptan(CH_(3)SH)with low power consumption is crucial for assessing air quality and facilitating non-invasive diagnosis of diseases such as periodontitis.Herein,we synthesized a ternary CeO_(2)-ZnO-Ag nanocomposite by a simple sol-gel one-step method,which shows the capability of monitoring ppb-level CH_(3)SH under room temperature.The incorporation of Ag significantly reduces the particle size and increases the ratio of Ce^(3+)as well as oxygen vacancy.Furthermore,Ag nanoparticles improve light utilization efficiency in CeO_(2)-ZnO composites in favor of the separation of photo-generated charge carriers.The sensor based on the nanocomposites with 2 mol%Ag exhibits an exceptional response of 1.21 towards 50 ppb CH3SH at room temperature under photoassisted excitation(395 nm).Moreover,it shows a stable detection even in an environment with 57.6% humidity and high selectivity towards CH_(3)SH gas.The gas sensing mechanism study indicates that the enhancement in perfo rmance is prima rily attributed to an increased number of oxygen vacancies and the spillover effect of Ag,ultimately leading to an augmented reaction rate of CH_(3)SH on the surface of the sensing material.This work demonstrates that the optimized CeO_(2)-ZnO-Ag nanocomposites hold great promise for highly selective and sensitive detection of trace CH_(3)SH gas under specific humidity conditions.展开更多
Microwave absorbing materials(MAMs)with wide effective absorption bandwidth(EAB)and low filling ratio are highly desirable for practical applications.Rational design in components and structures is one of the effectiv...Microwave absorbing materials(MAMs)with wide effective absorption bandwidth(EAB)and low filling ratio are highly desirable for practical applications.Rational design in components and structures is one of the effective strategies to achieve MAMs with high performance.Herein,double-shelled hollow(DSH)polypyrrole(PPy)nanotubes were synthesized with hydrochloric acid(HCl)and sodium pstyrene sulfonate(SS)co-doping polymerization process using manganese dioxide(MnO_(2))nanorods as a self-sacrifice template.With the increase of HCl concentration,the 1D MnO_(2) core diminishes gradually to form the MnO_(2)@PPy coaxial nanostructures and finally the DSH PPy nanotube,which tunes the microwave absorption performance.Importantly,the DSH PPy nanotubes exhibit excellent microwave absorption of an optimal reflection loss of–50.4 dB and a wide EAB of 7.7 GHz with a low filling ratio of 5 wt%in a paraffin wax matrix.The excellent microwave absorption is believed to be mainly attributed to the enhanced synergistic effects of interfacial polarization and conduction loss arising from the unique DSH structure and the co-doping polymerization.展开更多
Imaging-guided phototherapy holds promise for precision cancer treatment.However,most photosensitizers have only a singular modality of photodynamic therapy(PDT)or photothermal therapy(PTT),which make their therapeuti...Imaging-guided phototherapy holds promise for precision cancer treatment.However,most photosensitizers have only a singular modality of photodynamic therapy(PDT)or photothermal therapy(PTT),which make their therapeutic efficacy severely limited by the hypoxic and complex tumor microenvironment(TME).In this article,we provide a smart platform design(BOD-D)based on a visualized light-triggered phototherapeutic switch for transforming cancer therapy from near-infrared(NIR)-I imaging-guided PDT to activatable NIR-II-guided PTT while releasing nitric oxide(NO)for gas therapy(GT).BOD-D releases native NIR one-region fluorescence signals in tumors,which is used to direct robust PDT for tumor killing.As PDT is administered,the decreasing oxygen content in TME becomes progressively insufficient to maintain its excellent cell-killing effect.Subsequently,light triggers the dissociation of NO in BOD-D,activating a photothermal agent BOD-T that emits NIR-II fluorescence,for subsequent PTT.Notably,not only the light-mediated therapeutic mechanism can be switched from NIR-I-guided PDT to NIR-II-guided PTT,but also the NO released during this process will be used for GT to sensitize the above PDT and PTT.Our study contributes to the design of intelligent photosensitizers for cascade tumor photoablation.展开更多
Taking apart in numerous physiological and pathological activities,hydrogen sulfide(H_(2)S)has been selected as an excellent target spot for the early diagnosis of cancer.So far,there are many mature probes that apply...Taking apart in numerous physiological and pathological activities,hydrogen sulfide(H_(2)S)has been selected as an excellent target spot for the early diagnosis of cancer.So far,there are many mature probes that apply single optical imaging to monitor endogenous H_(2)S.Nevertheless,a single modality is not an ideal method to afford accurate diagnostic information in comprehensive biological organisms.Herein,we developed a dual-modal imaging probe BWS.This designed probe showed a specific response to H_(2)S with both chemiluminescence and NIR fluorescence light-up.The concurrence of fluorescence and chemiluminescence signal provided“double insurances”for highly accurate monitoring of H_(2)S.Satisfactorily,this dual-modal imaging probe performed precise visualization of endogenous H_(2)S in living cells and in vivo.We envisaged that this chemiluminescence/fluorescence real-time dual-modality strategy for H_(2)S detection will expand and optimize the multimodal imaging methods for efficient diagnosis and treatment of cancer.展开更多
Gas therapy(GT)combined with photodynamic therapy(PDT)is an effective strategy to compensate for the PDT limitation caused by the hypoxic tumor microenvironment,which can greatly improve PDT efficacy.The uncontrolled ...Gas therapy(GT)combined with photodynamic therapy(PDT)is an effective strategy to compensate for the PDT limitation caused by the hypoxic tumor microenvironment,which can greatly improve PDT efficacy.The uncontrolled leakage of gas molecules during delivery seriously hinders its practical biological application.Herein,we report a multifunction nanomedicine that enables precise gas therapy(including carbon monoxide(CO)release and H_(2)S depletion)using a multi-parameter-induced activation gas release strategy,enlarging the PDT efficacy.This nanomedicine uses a disulfide bond to covalently link a photosensitizer with the CO donor 3-hydroxyflavone(3-HF).The disulfide bond can be specifically consumed in H_(2)S-rich tumor areas,releasing the CO donor(3-HF),and also depleting H_(2)S.More importantly,the photo-controlled production of^(1)O_(2)can induce 3-HF precise release of CO in the tumor location.Such H_(2)S,light,and^(1)O_(2)multi-parameter-induced activation of gas release strategy ensures the accuracy of GT to amplify PDT efficiency.As expected,in vitro and in vivo investigations show that GT makes up for the PDT limitation,exhibiting the highest tumor therapeutic effect.This multi-parameter-activated design strategy provides a new way to improve the precision and efficacy of multimodal synergistic therapy of tumors.展开更多
Optical imaging with molecular probes is becoming an essential tool for advancing biological research and clinical applications.However,most currently available molecular probes show limited sensitivity,specificity,an...Optical imaging with molecular probes is becoming an essential tool for advancing biological research and clinical applications.However,most currently available molecular probes show limited sensitivity,specificity,and accuracy due to their typical responsiveness to a single stimulation for biomarker-based imaging.In this study,we develop a novel molecular probe that shows alkaline phosphatase(ALP)-instructed sensitive responsiveness to hydrogen sulfide for accurate cancer imaging and differentiation.This designed probe in an aggregated state under physiological conditions bears negatively charged surfaces,giving poor optical response to H_(2)S.The ALP-mediated dephosphorylation reaction yields an assembled product with a positively charged surface,affording significantly aggregation-enhanced responsiveness to H_(2)S with light-up NIR fluorescence at 755 nm.Such charge reversal of assembled probe from negative to positive plays a vital role in allowing precise visualization and differentiation of cancers based on differences in ALP upregulation and H_(2)S content.We envisage that our charge-reversal strategy for multiple-parameter-activated molecule probes will facilitate boosting the specificity and precision of cancer imaging.展开更多
基金Project supported by China Postdoctoral Science Foundation(2020M673172)National Natural Science Foundation of China(61901401)。
文摘The effective detection of trace methyl mercaptan(CH_(3)SH)with low power consumption is crucial for assessing air quality and facilitating non-invasive diagnosis of diseases such as periodontitis.Herein,we synthesized a ternary CeO_(2)-ZnO-Ag nanocomposite by a simple sol-gel one-step method,which shows the capability of monitoring ppb-level CH_(3)SH under room temperature.The incorporation of Ag significantly reduces the particle size and increases the ratio of Ce^(3+)as well as oxygen vacancy.Furthermore,Ag nanoparticles improve light utilization efficiency in CeO_(2)-ZnO composites in favor of the separation of photo-generated charge carriers.The sensor based on the nanocomposites with 2 mol%Ag exhibits an exceptional response of 1.21 towards 50 ppb CH3SH at room temperature under photoassisted excitation(395 nm).Moreover,it shows a stable detection even in an environment with 57.6% humidity and high selectivity towards CH_(3)SH gas.The gas sensing mechanism study indicates that the enhancement in perfo rmance is prima rily attributed to an increased number of oxygen vacancies and the spillover effect of Ag,ultimately leading to an augmented reaction rate of CH_(3)SH on the surface of the sensing material.This work demonstrates that the optimized CeO_(2)-ZnO-Ag nanocomposites hold great promise for highly selective and sensitive detection of trace CH_(3)SH gas under specific humidity conditions.
基金supported by the National Natural Science Foundation of China(No.22165032 and 22265031)the Applied Basic Research Fund of Yunnan Province(No.2019FB129)the Major Science and Technology Project of Precious Metal Materials Genetic Engineering in Yunnan Province(No.2021102AB080019-2)。
文摘Microwave absorbing materials(MAMs)with wide effective absorption bandwidth(EAB)and low filling ratio are highly desirable for practical applications.Rational design in components and structures is one of the effective strategies to achieve MAMs with high performance.Herein,double-shelled hollow(DSH)polypyrrole(PPy)nanotubes were synthesized with hydrochloric acid(HCl)and sodium pstyrene sulfonate(SS)co-doping polymerization process using manganese dioxide(MnO_(2))nanorods as a self-sacrifice template.With the increase of HCl concentration,the 1D MnO_(2) core diminishes gradually to form the MnO_(2)@PPy coaxial nanostructures and finally the DSH PPy nanotube,which tunes the microwave absorption performance.Importantly,the DSH PPy nanotubes exhibit excellent microwave absorption of an optimal reflection loss of–50.4 dB and a wide EAB of 7.7 GHz with a low filling ratio of 5 wt%in a paraffin wax matrix.The excellent microwave absorption is believed to be mainly attributed to the enhanced synergistic effects of interfacial polarization and conduction loss arising from the unique DSH structure and the co-doping polymerization.
基金supported by the National Natural Science Foundation of China(82173657,22077030,and 22271092)the Shanghai Municipal Science and Technology Major Project(2018SHZDZX03).
文摘Imaging-guided phototherapy holds promise for precision cancer treatment.However,most photosensitizers have only a singular modality of photodynamic therapy(PDT)or photothermal therapy(PTT),which make their therapeutic efficacy severely limited by the hypoxic and complex tumor microenvironment(TME).In this article,we provide a smart platform design(BOD-D)based on a visualized light-triggered phototherapeutic switch for transforming cancer therapy from near-infrared(NIR)-I imaging-guided PDT to activatable NIR-II-guided PTT while releasing nitric oxide(NO)for gas therapy(GT).BOD-D releases native NIR one-region fluorescence signals in tumors,which is used to direct robust PDT for tumor killing.As PDT is administered,the decreasing oxygen content in TME becomes progressively insufficient to maintain its excellent cell-killing effect.Subsequently,light triggers the dissociation of NO in BOD-D,activating a photothermal agent BOD-T that emits NIR-II fluorescence,for subsequent PTT.Notably,not only the light-mediated therapeutic mechanism can be switched from NIR-I-guided PDT to NIR-II-guided PTT,but also the NO released during this process will be used for GT to sensitize the above PDT and PTT.Our study contributes to the design of intelligent photosensitizers for cascade tumor photoablation.
基金supported by the National Natural Science Foundation of China(22077030,22271092,21977018,82173657)the China Postdoctoral Science Foundation(2021M701196)。
文摘Taking apart in numerous physiological and pathological activities,hydrogen sulfide(H_(2)S)has been selected as an excellent target spot for the early diagnosis of cancer.So far,there are many mature probes that apply single optical imaging to monitor endogenous H_(2)S.Nevertheless,a single modality is not an ideal method to afford accurate diagnostic information in comprehensive biological organisms.Herein,we developed a dual-modal imaging probe BWS.This designed probe showed a specific response to H_(2)S with both chemiluminescence and NIR fluorescence light-up.The concurrence of fluorescence and chemiluminescence signal provided“double insurances”for highly accurate monitoring of H_(2)S.Satisfactorily,this dual-modal imaging probe performed precise visualization of endogenous H_(2)S in living cells and in vivo.We envisaged that this chemiluminescence/fluorescence real-time dual-modality strategy for H_(2)S detection will expand and optimize the multimodal imaging methods for efficient diagnosis and treatment of cancer.
基金supported by the National Natural Science Foundation of China(22077030,22271092,21977018,82173657)the Shanghai Municipal Science and Technology Major Project(2018SHZDZX03)。
文摘Gas therapy(GT)combined with photodynamic therapy(PDT)is an effective strategy to compensate for the PDT limitation caused by the hypoxic tumor microenvironment,which can greatly improve PDT efficacy.The uncontrolled leakage of gas molecules during delivery seriously hinders its practical biological application.Herein,we report a multifunction nanomedicine that enables precise gas therapy(including carbon monoxide(CO)release and H_(2)S depletion)using a multi-parameter-induced activation gas release strategy,enlarging the PDT efficacy.This nanomedicine uses a disulfide bond to covalently link a photosensitizer with the CO donor 3-hydroxyflavone(3-HF).The disulfide bond can be specifically consumed in H_(2)S-rich tumor areas,releasing the CO donor(3-HF),and also depleting H_(2)S.More importantly,the photo-controlled production of^(1)O_(2)can induce 3-HF precise release of CO in the tumor location.Such H_(2)S,light,and^(1)O_(2)multi-parameter-induced activation of gas release strategy ensures the accuracy of GT to amplify PDT efficiency.As expected,in vitro and in vivo investigations show that GT makes up for the PDT limitation,exhibiting the highest tumor therapeutic effect.This multi-parameter-activated design strategy provides a new way to improve the precision and efficacy of multimodal synergistic therapy of tumors.
基金This research was made possible as a result of generous grants from the National Natural Science Foundation of China(grant nos.21874043,22077030,and 21977018)the Shanghai Municipal Science and Technology Major Project(grant no.2018SHZDZX03)the China Postdoctoral Science Foundation(grant no.2021M701196).
文摘Optical imaging with molecular probes is becoming an essential tool for advancing biological research and clinical applications.However,most currently available molecular probes show limited sensitivity,specificity,and accuracy due to their typical responsiveness to a single stimulation for biomarker-based imaging.In this study,we develop a novel molecular probe that shows alkaline phosphatase(ALP)-instructed sensitive responsiveness to hydrogen sulfide for accurate cancer imaging and differentiation.This designed probe in an aggregated state under physiological conditions bears negatively charged surfaces,giving poor optical response to H_(2)S.The ALP-mediated dephosphorylation reaction yields an assembled product with a positively charged surface,affording significantly aggregation-enhanced responsiveness to H_(2)S with light-up NIR fluorescence at 755 nm.Such charge reversal of assembled probe from negative to positive plays a vital role in allowing precise visualization and differentiation of cancers based on differences in ALP upregulation and H_(2)S content.We envisage that our charge-reversal strategy for multiple-parameter-activated molecule probes will facilitate boosting the specificity and precision of cancer imaging.
