Radiotherapy is an important treatment for cancer,but it is associated with major side effects due to the high dose of radiation(generally more than 50 Gy).Because radiation's low acute and late toxicity,many tumo...Radiotherapy is an important treatment for cancer,but it is associated with major side effects due to the high dose of radiation(generally more than 50 Gy).Because radiation's low acute and late toxicity,many tumors are treated with fractionated radiation in small doses(<2 Gy).Scintillator X-ray-induced photodynamic therapy is an efficient methodology for cancer management that employs small doses of X-ray irradiation(<2 Gy)in a complex process.Here we screened pharmaceutical drug intermediates that are derivatives of thioxanthone(TX)and investigated TX-derived organic pharmaceutical molecules that efficiently undergo X-ray-sensitization to populate triplet excitons(singlet oxygen)for cancer therapy when exposed to low-dose X-ray irradiation.By modifying alkoxy side chain substitutions at the 2-position to tune the molecular packing and intermolecular interactions,the fluorescence and room-temperature phosphorescence of a series of TX derivatives were assessed under X-ray irradiation.The ability of these derivatives to generate singlet oxygen and their potential for treating tumors provide new opportunities for developing organic molecules with simple chemical structures,in which large numbers of triplets can be populated directly under ultralow-dose X-ray irradiation.展开更多
Immobilizing enzymes within metal-organic frameworks(MOFs)enables enzymes to against extreme environments.However,these MOF shells are just like armors,protective but heavy,which shield the enzymes from threats while ...Immobilizing enzymes within metal-organic frameworks(MOFs)enables enzymes to against extreme environments.However,these MOF shells are just like armors,protective but heavy,which shield the enzymes from threats while locking them in the cage.The exploitation of immobilization strategy and intrinsic property of MOFs themselves is of great significance.Here,we proposed a functional protein trap strategy for efficient enzyme encapsulation.The ferrocenedicarboxylic acid(Fc)was used to induce the formation of defect-rich Co-based MOFs(CoBDC-Fc).As result,the engineered protein trap can not only improve the enzyme loading but also accelerate catalytic efficiency.Specifically,the atomically dispersed Fc sites serve as cocatalysts/cofactors and even change the conformation of enzymes in the construed microenvironment.Furthermore,the obtained CoBDC-Fc/enzyme exhibits excellent recyclability and tolerance to inhospitable conditions.Benefited by these,the CoBDC-Fc/enzyme/antigen composites were further prepared for cascade enzyme-linked immunosorbent assay of prostate-specific antigen with satisfactory sensitivity.展开更多
Achieving high-efficiency deep blue emitter with CIE_(y)<0.06(CIE,Commission Internationale de L’Eclairage)and external quantum efficiency(EQE)>10%has been a long-standing challenge for traditional fluorescent ...Achieving high-efficiency deep blue emitter with CIE_(y)<0.06(CIE,Commission Internationale de L’Eclairage)and external quantum efficiency(EQE)>10%has been a long-standing challenge for traditional fluorescent materials in organic light-emitting diodes(OLEDs).Here,we report the rational design and synthesis of two new deep blue luminogens:4-(10-(4’-(9 H-carbazol-9-yl)-2,5-dimethyl-[1,1’-biphe nyl]-4-yl)anthracen-9-yl)benzonitrile(2 M-ph-pCzAnBzt)and 4-(10-(4-(9 H-carbazol-9-yl)-2,5-dimethyl phenyl)anthracen-9-yl)benzonitrile(2 M-pCzAnBzt).In particular,2 M-ph-pCzAnBzt produces saturated deep blue emissions in a non-doped electroluminescent device with an exceptionally high EQE of 10.44% and CIE_(x,y)(0.151,0.057).The unprecedented electroluminescent efficiency is attributed to the combined effects of higher-order reversed intersystem crossing and triplet-triplet up-conversion,which are supported by analysis of theoretical calculation,triplet sensitization experiments,as well as nanosecond transient absorption spectroscopy.This research offers a new approach to resolve the shortage of high efficiency deep blue fluorescent emitters.展开更多
In order to develop pure organic single-molecule white-light emitters(SMWLE),the oxidation of thianthrene(TA)was performed on sulfur atoms at different degrees to tune room temperature phosphorescence(RTP)emission.Wit...In order to develop pure organic single-molecule white-light emitters(SMWLE),the oxidation of thianthrene(TA)was performed on sulfur atoms at different degrees to tune room temperature phosphorescence(RTP)emission.With increasing degrees of oxidation from 1OTA,2OTA,3OTA,to 4OTA,monomeric and aggregative RTP emission was gradually suppressed,due to the gradual disappearance of lone pair electrons on sulfur atoms.Among these compounds,monomers and aggregates of 1OTA demonstrated a better intensity match between fluorescence and RTP.展开更多
A reversible dual-responsive luminescent material was introduced by our group to show the simultaneous color and lifetime switching in response to external stimuli.Pristine crystalline powder of(E)-2-(benzo[d]thiazol-...A reversible dual-responsive luminescent material was introduced by our group to show the simultaneous color and lifetime switching in response to external stimuli.Pristine crystalline powder of(E)-2-(benzo[d]thiazol-2-yl)-3-(pyren-1-yl)acrylonitrile(Py-BZTCN)shows the orderedπ–πstacking with only near-monomer-normal orange-yellow fluorescence,but it exhibits red emission with thermally activated delayed fluorescence(TADF)after grinding,which can be reversibly recovered by heating or fuming treatment.Grinding disturbs the orderedπ–πstacking of pristine powder,leading to the formation of small aggregates with compressed distance and increased overlap ofπ–πstacking between adjacent molecules.The cause of switching was verified by single-crystal X-ray diffraction experiments of two corresponding crystals.This strongπ–πinteraction effectively promotes the excited-state energy splitting and substantially decreases the singlet–triplet energy gap(ΔEST)of aggregates,resulting in the red TADF emission of aggregates through reverse intersystem crossing.This finding proposes a new route to realizing the TADF emission of aggregates through strong intermolecular interactions based on non-TADF monomer,thereby enabling a novel high-contrast dualresponsive luminescence switching.展开更多
基金supported by the National Natural Science Foundation of China(82172007,81771977,52103209,and 52373183)the Science Fund for Distinguished Young Scholars of Fujian Province(2021J06007)+2 种基金the Scientific Research Foundation of Xiang An Biomedicine Laboratory(2023XAKJ0101023)the Open Research Fund of the National Facility for Translational Medicine(Shanghai)(TMSK-2021-102)the Open Project of State Key Laboratory of Supramolecular Structure and Materials(sklssm2023026)。
文摘Radiotherapy is an important treatment for cancer,but it is associated with major side effects due to the high dose of radiation(generally more than 50 Gy).Because radiation's low acute and late toxicity,many tumors are treated with fractionated radiation in small doses(<2 Gy).Scintillator X-ray-induced photodynamic therapy is an efficient methodology for cancer management that employs small doses of X-ray irradiation(<2 Gy)in a complex process.Here we screened pharmaceutical drug intermediates that are derivatives of thioxanthone(TX)and investigated TX-derived organic pharmaceutical molecules that efficiently undergo X-ray-sensitization to populate triplet excitons(singlet oxygen)for cancer therapy when exposed to low-dose X-ray irradiation.By modifying alkoxy side chain substitutions at the 2-position to tune the molecular packing and intermolecular interactions,the fluorescence and room-temperature phosphorescence of a series of TX derivatives were assessed under X-ray irradiation.The ability of these derivatives to generate singlet oxygen and their potential for treating tumors provide new opportunities for developing organic molecules with simple chemical structures,in which large numbers of triplets can be populated directly under ultralow-dose X-ray irradiation.
基金support of the National Natural Science Foundation of China(Nos.22074049 and 22004042)the Fundamental Research Funds for the Central Universities(No.CCNU22JC006)the Program of Introducing Talents of Discipline to Universities of China(111 program,No.B17019).
文摘Immobilizing enzymes within metal-organic frameworks(MOFs)enables enzymes to against extreme environments.However,these MOF shells are just like armors,protective but heavy,which shield the enzymes from threats while locking them in the cage.The exploitation of immobilization strategy and intrinsic property of MOFs themselves is of great significance.Here,we proposed a functional protein trap strategy for efficient enzyme encapsulation.The ferrocenedicarboxylic acid(Fc)was used to induce the formation of defect-rich Co-based MOFs(CoBDC-Fc).As result,the engineered protein trap can not only improve the enzyme loading but also accelerate catalytic efficiency.Specifically,the atomically dispersed Fc sites serve as cocatalysts/cofactors and even change the conformation of enzymes in the construed microenvironment.Furthermore,the obtained CoBDC-Fc/enzyme exhibits excellent recyclability and tolerance to inhospitable conditions.Benefited by these,the CoBDC-Fc/enzyme/antigen composites were further prepared for cascade enzyme-linked immunosorbent assay of prostate-specific antigen with satisfactory sensitivity.
基金supported by the National Natural Science Foundation of China(62004074,51727809)the Science and Technology Department of Hubei Province(2019AAA063,2020BAA016)。
文摘Achieving high-efficiency deep blue emitter with CIE_(y)<0.06(CIE,Commission Internationale de L’Eclairage)and external quantum efficiency(EQE)>10%has been a long-standing challenge for traditional fluorescent materials in organic light-emitting diodes(OLEDs).Here,we report the rational design and synthesis of two new deep blue luminogens:4-(10-(4’-(9 H-carbazol-9-yl)-2,5-dimethyl-[1,1’-biphe nyl]-4-yl)anthracen-9-yl)benzonitrile(2 M-ph-pCzAnBzt)and 4-(10-(4-(9 H-carbazol-9-yl)-2,5-dimethyl phenyl)anthracen-9-yl)benzonitrile(2 M-pCzAnBzt).In particular,2 M-ph-pCzAnBzt produces saturated deep blue emissions in a non-doped electroluminescent device with an exceptionally high EQE of 10.44% and CIE_(x,y)(0.151,0.057).The unprecedented electroluminescent efficiency is attributed to the combined effects of higher-order reversed intersystem crossing and triplet-triplet up-conversion,which are supported by analysis of theoretical calculation,triplet sensitization experiments,as well as nanosecond transient absorption spectroscopy.This research offers a new approach to resolve the shortage of high efficiency deep blue fluorescent emitters.
基金supported by the National Natural Science Foundation of China(51873077,91833304,and 51803071)the National Basic Research Program of China(2016YFB0401001)+1 种基金the Postdoctoral Innovation Talent Support Project(BX20180121)the China Postdoctoral Science Foundation(2018M641767),and JLUSTIRT(2019TD-33).
文摘In order to develop pure organic single-molecule white-light emitters(SMWLE),the oxidation of thianthrene(TA)was performed on sulfur atoms at different degrees to tune room temperature phosphorescence(RTP)emission.With increasing degrees of oxidation from 1OTA,2OTA,3OTA,to 4OTA,monomeric and aggregative RTP emission was gradually suppressed,due to the gradual disappearance of lone pair electrons on sulfur atoms.Among these compounds,monomers and aggregates of 1OTA demonstrated a better intensity match between fluorescence and RTP.
基金supported by the National Natural Science Foundation of China(nos.52073117,91833304,51873077,and 51803071)the National Basic Research Program of China(no.2016YFB0401001)+1 种基金the Postdoctoral Innovation Talent Support Project(no.BX20180121)the China Postdoctoral Science Foundation(nos.2018M641767 and 2019TQ0198).
文摘A reversible dual-responsive luminescent material was introduced by our group to show the simultaneous color and lifetime switching in response to external stimuli.Pristine crystalline powder of(E)-2-(benzo[d]thiazol-2-yl)-3-(pyren-1-yl)acrylonitrile(Py-BZTCN)shows the orderedπ–πstacking with only near-monomer-normal orange-yellow fluorescence,but it exhibits red emission with thermally activated delayed fluorescence(TADF)after grinding,which can be reversibly recovered by heating or fuming treatment.Grinding disturbs the orderedπ–πstacking of pristine powder,leading to the formation of small aggregates with compressed distance and increased overlap ofπ–πstacking between adjacent molecules.The cause of switching was verified by single-crystal X-ray diffraction experiments of two corresponding crystals.This strongπ–πinteraction effectively promotes the excited-state energy splitting and substantially decreases the singlet–triplet energy gap(ΔEST)of aggregates,resulting in the red TADF emission of aggregates through reverse intersystem crossing.This finding proposes a new route to realizing the TADF emission of aggregates through strong intermolecular interactions based on non-TADF monomer,thereby enabling a novel high-contrast dualresponsive luminescence switching.
