Herein,we report a new metal-organic framework with an AIE ligand (H_(4)TCPP=2,3,5,6-tetra-(4-carboxyphenyl)pyrazine) and Mg^(2+) ions,that is,[Mg_(2)(H_(2)O)_(4)TCPP]·DMF·5CH_(3)CN (Mg-TCPP,TCPP=tetra-(4-ca...Herein,we report a new metal-organic framework with an AIE ligand (H_(4)TCPP=2,3,5,6-tetra-(4-carboxyphenyl)pyrazine) and Mg^(2+) ions,that is,[Mg_(2)(H_(2)O)_(4)TCPP]·DMF·5CH_(3)CN (Mg-TCPP,TCPP=tetra-(4-carboxyphenyl)pyrazine) for detection of nitroaromatic explosives.Due to the coordination effect and restricted intramolecular rotation,Mg-TCPP exhibits bright blue light.As a fluorescent sensor,Mg-TCPP exhibits high selectivity and sensitivity for sensing 2,4,6-trinitrophenol (TNP) by quenching behaviors with the Stern-Volmer quenching constant (K_(SV)) of 3.63×10^(5)L/mol and achieves the low limit of detection of 25.6 ppb,which is beyond most of the previously reported fluorescent materials.Notably,the portable Mg-TCPP films are prepared and it can be used for rapid and sensitive TNP detection in a variety of environments including organic solvent and aqueous solution.Moreover,TNP vapor can be detected within 3 min by naked eye and the film could be regenerated under simple solvent cleaning.展开更多
Luminescent polymers have garnered considerable research attention for their excellent properties and wide range of applications in multi-responsive materials,bioimaging,and photoelectric devices.Thereout,various modu...Luminescent polymers have garnered considerable research attention for their excellent properties and wide range of applications in multi-responsive materials,bioimaging,and photoelectric devices.Thereout,various modulations of polymer structure are often the main approach to obtaining materials with different luminescent colors and functions.However,polymers with biodegradability,tunable color,and efficient emission simultaneously remain a challenge.Herein,we report a feasible strategy to achieve degradable and highly emissive polymers by exquisite combination and interplay of aggregation-induced emission(AIE)unit and environmental-friendly epoxide/CO_(2)copolymerization.A series of polycarbonates P-TEP_(x)CN_(y)(x=0,1,2,4,30,120;y=0,1)were prepared,with emission color changed from blue to yellow by controlling the proportion of two designed AIE-active monomers.Among them,Using P-TCN as emitting layer,high performance white light-emitting diode(WLED)device with an external quantum efficiency(EQE)of 26.09%and CIE coordinates of(0.32,0.32)was achieved.In addition,the designed polymers can be used as selective sensors for nitroaromatic compounds in their nanoaggregate states.展开更多
Chirality is one of the most important features of the nature.The recognition of enantiomers plays significant roles in the field of life science,pharmaceutical analysis and food chemistry.Among various recognition me...Chirality is one of the most important features of the nature.The recognition of enantiomers plays significant roles in the field of life science,pharmaceutical analysis and food chemistry.Among various recognition methods,fluorescence spectrometry has attracted much attention of researchers thanks to its high sensitivity and easy operation.Compared with traditional fluorescent probes,chiral molecules with aggregation-induced emission(AIE)have drawn increasing interests due to their huge potential in high-efficiency chemo/biosensors and solid emitters.Chiral AIE luminogens(AIEgens)can not only discriminate two enantiomers with excellent enantioselectivity,but also show general applicability for many chiral analytes,such as chiral acids,amino acids,amines,alcohols.In this review,we mainly summarized the recent development of chiral probes with AIE properties,including chiral tetraphenylethylene(TPE)derivatives,α-cyanostilbene derivatives,Schiff base derivatives and other AIEgens.Their synthetic routes,recognition capabilities and possible working mechanisms were well discussed.It is envisioned that the present review can give some significant guidance for design and synthesis of chiral AIEgens with good enantioselectivity and inspire more readers to join the research of chiral AIE.展开更多
Dual-state emission(DSE)molecules displayed conspicuous fluorescent performance both in solid and solution states.However,the construction of DSE molecules and the regulation of their emission wavelengths remains a gr...Dual-state emission(DSE)molecules displayed conspicuous fluorescent performance both in solid and solution states.However,the construction of DSE molecules and the regulation of their emission wavelengths remains a great challenge.Based on the structure-function relationship of quinolinonitrile-type fluorophores,this work proposed a feasible strategy for modulating their fluorescent properties into DSE via limiting the torsion angle between the quinoline ring and C=C bond in the range of 4.7°to 30°.Based on this strategy,53 compounds were obtained which displayed tunable emission wavelengths from^(3)97 nm to 740 nm in solid-state and from 360 nm to 672 nm in solution.The feasibility of the strategy was supported by a series of theoretical calculations,optical characterizations,and crystal analysis,suggesting the compounds have great potential in imaging living cells and tissues with desired wavelengths.展开更多
Hypoxia is a significant feature in most of solid tumors.Hence;developing hypoxia-responsive phototheranostic system is still a challenge.In this contribution;a supramolecular assembly strategy based on sulfonate-func...Hypoxia is a significant feature in most of solid tumors.Hence;developing hypoxia-responsive phototheranostic system is still a challenge.In this contribution;a supramolecular assembly strategy based on sulfonate-functionalized azocalix[4]arene(SAC4A)and cationic aggregation-induced emission photosensitizer(namely TPA-H)was proposed for hypoxia-responsive bioimaging and photodynamic therapy(PDT).Upon supramolecular complexation of TPA-H and SAC4A through electrostatic interaction;the fluorescence and reactive oxygen species(ROS)generation of TPA-H were largely inhibited.In hypoxic tumors;the azo group of SAC4A can be reduced to aniline derivative and release the included TPA-H to recover its pristine fluorescence and ROS.Interestingly;the free TPA-H undergoes cell membrane-to-mitochondria translocation during cell imaging;achieving a real-time self-reporting PDT system.In vivo tumor imaging and therapy reveal that this as-prepared supramolecular complexes have good biosafety and efficient antitumor activity under hypoxia.Such hypoxia-responsive supramolecular photosensitizer system will enrich image-guided photodynamic therapy.展开更多
Supramolecular assembly based on efficient Förster resonance energy transfer(FRET)provides an optimal framework for the development of substantial artificial light-harvesting systems(LHSs).In this study,a sequent...Supramolecular assembly based on efficient Förster resonance energy transfer(FRET)provides an optimal framework for the development of substantial artificial light-harvesting systems(LHSs).In this study,a sequential two-step light-harvesting system with FRET process was successfully established in aqueous medium where a specially designed deep blue-emitting indole derivative(PZ)served as an energy donor,a novel green-emitting tetraphenylethylene-based tricycle(TPEM)with aggregation-induced emission(AIE)functioned as a relay acceptor,and Nile red(NIR)was used as the terminal acceptor.Due to good spectral overlap and close proximity between donors and acceptors,the triad system(PZ/TPEM/NIR)could allow for significant energy transfer from PZ to TPEM to NIR with a ratio of 1000:40:30,affording very high energy-transfer efficiencies(Φ_(ET))of 98.59%.By properly optimizing the proportion of PZ/TPEM/NIR,bright white light emission was readily obtained with a CIE coordinate of(0.32,0.33).Significantly,undesired fluorescence quenching was effectively circumvented in the TPEM-based FRET process.The captured solar energy by PZ/TPEM/NIR assemblies can further photocatalyze the Knoevenagel condensation reaction with a high yield of 95%under visible light in an aqueous medium.Therefore,the tunable feature of the supramolecular strategy renders the AIEgen-based macrocycle a highly promising candidate to construct efficient LHSs for photocatalysis.展开更多
Despite the rapid development of probes for targeting single organelle, the construction of robust dual-organelle targeting probes with multicolor emission was rarely reported. Herein, two dual-emissive aggregation-in...Despite the rapid development of probes for targeting single organelle, the construction of robust dual-organelle targeting probes with multicolor emission was rarely reported. Herein, two dual-emissive aggregation-induced emission luminogens(AIEgens)with donor-π-acceptor structures were designed and synthesized, namely QT-1 and QF-2. Both two AIEgens exhibited excitation wavelength-dependence defying the Kasha's rule, and could stain lipid droplets(LDs) and mitochondria in blue and red fluorescence, respectively. Moreover, thanks to the near-infrared emission and abundant reactive oxygen species(ROS) generation efficiency of QT-1, it was chosen as a photodynamic therapy agent to selectively kill cancer cells from normal cells. Upon light irradiation, an obvious decrease of mitochondrial membrane potential(MMP) and serious change of mitochondrial shape in cells were observed, which corresponded to the efficient inhibition of tumor growth in vivo. This work afforded a promising strategy for the construction of multicolor emission by tuning anti-Kasha behaviors and expanding their application in dualorganelle targeting-based phototheranostics.展开更多
Tetraphenylpyrazine(TPP)is a promising heterocycle-based aggregation-induced emission luminogen(AIEgen)which has sparked multiple applications in organic light-emitting diodes,sensors,and biotherapy.However,the utilit...Tetraphenylpyrazine(TPP)is a promising heterocycle-based aggregation-induced emission luminogen(AIEgen)which has sparked multiple applications in organic light-emitting diodes,sensors,and biotherapy.However,the utility of it in developing information storage materials is relatively rare.Moreover,TPP is mostly employed as an electronic acceptor in molecular design,while the consideration of it as an electronic donor is attractive in studies which may provide a full understanding of its property to tailor the materials.In this work,we synthesize three TPP-based molecules by decorating it with acrylonitrile and isomeric pyridine units,which show AIE behavior by property inheritance from their parent unit.Interestingly,the effective intramolecular charge transfer takes place from the TPP electronic donor to the acrylonitrile and pyridine electronic acceptor,therefore inducing a remarkable solvatochromic effect as the solvent polarity improves.Moreover,it is revealed that the isomeric effect of the nitrogen atom in the pyridines may pose an influence on the absorption,solvatochromism,and AIE behavior.In addition,the acrylonitrile and pyridine groups are reactive to light and acid-base stimuli with irreversible and reversible responses,respectively.Combined with the high light-harvesting ability of these AIEgens,they show great potential in the stimuli-responsive materials for dual information storage.展开更多
To meet the high requirements of biomedical applications in antimicrobial agents, it is crucial to explore efficient nanoantimicrobialagents with no resistance and good biocompatibility for treating infected wounds. I...To meet the high requirements of biomedical applications in antimicrobial agents, it is crucial to explore efficient nanoantimicrobialagents with no resistance and good biocompatibility for treating infected wounds. In this study, compositenano-antibiotic TPA-Py@AuNCs⊂BSA nanoparticles (TAB NPs) are prepared using hollow mesoporous Au nanocages (AuNCs)loaded with a photosensitizer (namely TPA-Py) with D-π-A structure showing aggregation-induced emission properties. WhenTPA-Py is encapsulated in the cavity of AuNCs, its fluorescence is suppressed. In the presence of photothermal induction, TPA-Pycan be released from the AuNCs, allowing for the restoration of fluorescence illumination and the specific imaging of Grampositivebacteria. TAB NPs demonstrate outstanding antimicrobial activity against a variety of bacteria, and this multimodalantimicrobial property does not lead to the development of bacterial resistance. In vitro experiments show that TAB NPs couldeliminate bacteria and ablate bacterial biofilm. In vivo experiments show that the synergistic antimicrobial effect of TAB NPs has asignificant positive impact on the treatment of infectedwounds, including rapid antibacterial action, promotion of M2 macrophagepolarization, and enhancement of chronic wound healing. This study provides an effective strategy for developing wide-spectrumnano-antibiotics for the ablation of bacterial biofilms and the treatment of infected wounds.展开更多
Solar-driven interfacial evaporation is a promising technology for desalination.The photothermal conversion materials are at the core and play a key role in thisfield.Design of photothermal conversion materials based ...Solar-driven interfacial evaporation is a promising technology for desalination.The photothermal conversion materials are at the core and play a key role in thisfield.Design of photothermal conversion materials based on organic dyes for desalina-tion is still a challenge due to lack of efficient guiding strategy.Herein,a new D(donor)-A(acceptor)type conjugated tetraphenylpyrazine(TPP)luminophore(namely TPP-2IND)was prepared as a photothermal conversion molecule.It exhib-ited a broad absorption spectrum and strongπ–πstacking in the solid state,resulting in efficient sunlight harvesting and boosting nonradiative decay.TPP-2IND powder exhibited high photothermal efficiency upon 660 nm laser irradiation(0.9 W cm^(-2)),and the surface temperature can reach to 200℃.Then,an interfacial heating system based on TPP-2IND is established successfully.The water evaporation rate and the solar-driven water evaporation efficiency were evaluated up to 1.04 kg m^(-2) h^(-1) and 65.8%under 1 sunlight,respectively.Thus,this novel solar-driven heating system shows high potential for desalination and stimulates the development of advanced photothermal conversion materials.展开更多
Enantioselective recognition and separation are the most important issues in the fields of chemistry,pharmacy,agrochemical,and food science.Here,we developed two optically active diamines showing aggregation-induced e...Enantioselective recognition and separation are the most important issues in the fields of chemistry,pharmacy,agrochemical,and food science.Here,we developed two optically active diamines showing aggregation-induced emission(AIE)that can discriminate 5 kinds of chiral acids with high enantioselectivity.Especially,a very high fluorescence intensity ratio(IL/ID)of 281 for(±)-Dibenzoyl-D/L-tartaric acid was obtained through the collection of fluorescence change after interaction with chiral AIE-active diamine.By virtue of AIE property and intermolecular acidbase interaction,enantioselective separation was facilely realized by simple filtration of the precipitates formed by chiral AIE luminogen(AIEgen)and one enantiomer in the racemic solution.The chiral HPLC data indicated that the precipitates of AIEgen/chiral acid possessed 82%L-analyte(the enantiomeric excess value was assessed to be 64%ee).Therefore,this method can serve as a simple,convenient,and low-cost tool for chiral detection and separation.展开更多
Organic reactions in water have attracted great attention due to their advantages such as unique reaction performance and environmental friendliness.Organic reactions as well as polymerizations in aqueous media have b...Organic reactions in water have attracted great attention due to their advantages such as unique reaction performance and environmental friendliness.Organic reactions as well as polymerizations in aqueous media have been extensively investigated,and so far,there has been a massive amount of reporting about polymerizations in water.However,reports about click polymerization in water have been rare.Herein,click polymerization of activated alkyne and aromatic amine in aqueous media is developed.The“on water”effect facilitates polymerization in aqueous media better than in organic solvents,and its mechanism is deciphered through experimental data and theoretical calculations.Water participates in the reaction and reduces the energy barrier to some extent.Besides,polymerization makes it possible for aromatic amine with low reactivity to be linked.By using this strategy,polymers with high molecular weights can be obtained in high yields(up to 95.4%).They show good thermal stability and high refractivity.They can be photodegraded.The polymers with tetraphenylethylene moieties show aggregation-induced emission and can be used as materials for generating photopatterns and visualizing agents for specific staining of lysosome in living cells.展开更多
基金supported by the National Natural Science Foundation of China(No.22175033)Science and Technology Development Plan of Jilin Province(Nos.YDZJ202101ZYTS063,20210508022RQ)Research Foundation of Education Department of Shaanxi Province(No.18JS009)。
文摘Herein,we report a new metal-organic framework with an AIE ligand (H_(4)TCPP=2,3,5,6-tetra-(4-carboxyphenyl)pyrazine) and Mg^(2+) ions,that is,[Mg_(2)(H_(2)O)_(4)TCPP]·DMF·5CH_(3)CN (Mg-TCPP,TCPP=tetra-(4-carboxyphenyl)pyrazine) for detection of nitroaromatic explosives.Due to the coordination effect and restricted intramolecular rotation,Mg-TCPP exhibits bright blue light.As a fluorescent sensor,Mg-TCPP exhibits high selectivity and sensitivity for sensing 2,4,6-trinitrophenol (TNP) by quenching behaviors with the Stern-Volmer quenching constant (K_(SV)) of 3.63×10^(5)L/mol and achieves the low limit of detection of 25.6 ppb,which is beyond most of the previously reported fluorescent materials.Notably,the portable Mg-TCPP films are prepared and it can be used for rapid and sensitive TNP detection in a variety of environments including organic solvent and aqueous solution.Moreover,TNP vapor can be detected within 3 min by naked eye and the film could be regenerated under simple solvent cleaning.
基金supported by the National Natural Science Foundation of China(No.22175033)the Scientific and Technological Innovation Team of Shanxi Province(No.2022TD-36).
文摘Luminescent polymers have garnered considerable research attention for their excellent properties and wide range of applications in multi-responsive materials,bioimaging,and photoelectric devices.Thereout,various modulations of polymer structure are often the main approach to obtaining materials with different luminescent colors and functions.However,polymers with biodegradability,tunable color,and efficient emission simultaneously remain a challenge.Herein,we report a feasible strategy to achieve degradable and highly emissive polymers by exquisite combination and interplay of aggregation-induced emission(AIE)unit and environmental-friendly epoxide/CO_(2)copolymerization.A series of polycarbonates P-TEP_(x)CN_(y)(x=0,1,2,4,30,120;y=0,1)were prepared,with emission color changed from blue to yellow by controlling the proportion of two designed AIE-active monomers.Among them,Using P-TCN as emitting layer,high performance white light-emitting diode(WLED)device with an external quantum efficiency(EQE)of 26.09%and CIE coordinates of(0.32,0.32)was achieved.In addition,the designed polymers can be used as selective sensors for nitroaromatic compounds in their nanoaggregate states.
基金partially supported by the National Natural Science Foundation of China(Nos.52173152,21805002)Guangdong Basic and Applied Basic Research Foundation(No.2020A1515110476)+2 种基金the Fund of the Rising Stars of Shaanxi Province(No.2021KJXX-48)Scientific and Technological Innovation Team of Shaanxi Province(No.2022TD-36)Scientific Research Program Funded by Shaanxi Provincial Education Department(No.22JK0247)。
文摘Chirality is one of the most important features of the nature.The recognition of enantiomers plays significant roles in the field of life science,pharmaceutical analysis and food chemistry.Among various recognition methods,fluorescence spectrometry has attracted much attention of researchers thanks to its high sensitivity and easy operation.Compared with traditional fluorescent probes,chiral molecules with aggregation-induced emission(AIE)have drawn increasing interests due to their huge potential in high-efficiency chemo/biosensors and solid emitters.Chiral AIE luminogens(AIEgens)can not only discriminate two enantiomers with excellent enantioselectivity,but also show general applicability for many chiral analytes,such as chiral acids,amino acids,amines,alcohols.In this review,we mainly summarized the recent development of chiral probes with AIE properties,including chiral tetraphenylethylene(TPE)derivatives,α-cyanostilbene derivatives,Schiff base derivatives and other AIEgens.Their synthetic routes,recognition capabilities and possible working mechanisms were well discussed.It is envisioned that the present review can give some significant guidance for design and synthesis of chiral AIEgens with good enantioselectivity and inspire more readers to join the research of chiral AIE.
基金supported by the National Natural Science Foundation of China(Nos.22077099 and 22171223)The Innovation Capability Support Program of Shaanxi(Nos.2023-CX-TD-75 and 2022KJXX-32)+5 种基金the Scientific and Technological Innovation Team of Shaanxi Province(No.2022TD-36)the Technology Innovation Leading Program of Shaanxi(No.2023KXJ-209)the Natural Science Basic Research Program of Shaanxi(Nos.2023-JC-YB-141 and 2022JQ-151)Young Talent Fund of Association for Science and Technology in Shaanxi,China(No.SWYY202206)the Shaanxi Fundamental Science Research Project for Chemistry&Biology(Nos.22JHZ010 and 22JHQ080)the Yan’an City Science and Technology Project(No.2022SLZDCY-002)。
文摘Dual-state emission(DSE)molecules displayed conspicuous fluorescent performance both in solid and solution states.However,the construction of DSE molecules and the regulation of their emission wavelengths remains a great challenge.Based on the structure-function relationship of quinolinonitrile-type fluorophores,this work proposed a feasible strategy for modulating their fluorescent properties into DSE via limiting the torsion angle between the quinoline ring and C=C bond in the range of 4.7°to 30°.Based on this strategy,53 compounds were obtained which displayed tunable emission wavelengths from^(3)97 nm to 740 nm in solid-state and from 360 nm to 672 nm in solution.The feasibility of the strategy was supported by a series of theoretical calculations,optical characterizations,and crystal analysis,suggesting the compounds have great potential in imaging living cells and tissues with desired wavelengths.
基金supported by the National Natural Science Foundation of China(52173152 and 21805002)the Fund of the Rising Stars of Shaanxi Province(2021KJXX-48)+2 种基金the Research Foundation of Education Department of Shaanxi Province(21JK0487)the Young Talent Fund of University Association for Science and Technology in Shaanxi,China(20190610 and 20210606)the Scientific and Technological Innovation Team of Shaanxi Province(2022TD-36).
文摘Hypoxia is a significant feature in most of solid tumors.Hence;developing hypoxia-responsive phototheranostic system is still a challenge.In this contribution;a supramolecular assembly strategy based on sulfonate-functionalized azocalix[4]arene(SAC4A)and cationic aggregation-induced emission photosensitizer(namely TPA-H)was proposed for hypoxia-responsive bioimaging and photodynamic therapy(PDT).Upon supramolecular complexation of TPA-H and SAC4A through electrostatic interaction;the fluorescence and reactive oxygen species(ROS)generation of TPA-H were largely inhibited.In hypoxic tumors;the azo group of SAC4A can be reduced to aniline derivative and release the included TPA-H to recover its pristine fluorescence and ROS.Interestingly;the free TPA-H undergoes cell membrane-to-mitochondria translocation during cell imaging;achieving a real-time self-reporting PDT system.In vivo tumor imaging and therapy reveal that this as-prepared supramolecular complexes have good biosafety and efficient antitumor activity under hypoxia.Such hypoxia-responsive supramolecular photosensitizer system will enrich image-guided photodynamic therapy.
基金supported by the National Natural Science Foundation of China(52173152)the Fund of the Rising Stars of Shaanxi Province(2021KJXX-48)+3 种基金the Research Foundation of Education Department of Shaanxi Province(21JK0487)the Scientific and Technological Innovation Team of Shaanxi Province(2022TD-36)the Natural Science Basic Research Plan in Shaanxi Province of China(2024JC-YBMS-123)the Industrial Science and Technology Plan in Shaanxi Provincial Education Department(23JC001)。
文摘Supramolecular assembly based on efficient Förster resonance energy transfer(FRET)provides an optimal framework for the development of substantial artificial light-harvesting systems(LHSs).In this study,a sequential two-step light-harvesting system with FRET process was successfully established in aqueous medium where a specially designed deep blue-emitting indole derivative(PZ)served as an energy donor,a novel green-emitting tetraphenylethylene-based tricycle(TPEM)with aggregation-induced emission(AIE)functioned as a relay acceptor,and Nile red(NIR)was used as the terminal acceptor.Due to good spectral overlap and close proximity between donors and acceptors,the triad system(PZ/TPEM/NIR)could allow for significant energy transfer from PZ to TPEM to NIR with a ratio of 1000:40:30,affording very high energy-transfer efficiencies(Φ_(ET))of 98.59%.By properly optimizing the proportion of PZ/TPEM/NIR,bright white light emission was readily obtained with a CIE coordinate of(0.32,0.33).Significantly,undesired fluorescence quenching was effectively circumvented in the TPEM-based FRET process.The captured solar energy by PZ/TPEM/NIR assemblies can further photocatalyze the Knoevenagel condensation reaction with a high yield of 95%under visible light in an aqueous medium.Therefore,the tunable feature of the supramolecular strategy renders the AIEgen-based macrocycle a highly promising candidate to construct efficient LHSs for photocatalysis.
基金supported by the National Natural Science Foundation of China (52173152, 21805002)Guangdong Basic and Applied Basic Research Foundation (2020A1515110476)+7 种基金the Fund of the Rising Stars of Shaanxi Province (2021KJXX-48)the Shenzhen Science and Technology Program (KQTD20210811090115019)the Major Instrumentation Development Program of the Chinese Academy of Sciences(ZDKYYQ20220008)Shenzhen Basic Research (key project)(China)(JCYJ20210324120011030)the Scientific and Technological Innovation Team of Shaanxi Province (2022TD-36)the National Key R&D Programs(China)(2021YFA0910001)Shaanxi Fundamental Science Research Project for Chemistry&Biology (22JHQ078)the Scientific Research Program Funded by Shaanxi Provincial Education Department (22JK0247)。
文摘Despite the rapid development of probes for targeting single organelle, the construction of robust dual-organelle targeting probes with multicolor emission was rarely reported. Herein, two dual-emissive aggregation-induced emission luminogens(AIEgens)with donor-π-acceptor structures were designed and synthesized, namely QT-1 and QF-2. Both two AIEgens exhibited excitation wavelength-dependence defying the Kasha's rule, and could stain lipid droplets(LDs) and mitochondria in blue and red fluorescence, respectively. Moreover, thanks to the near-infrared emission and abundant reactive oxygen species(ROS) generation efficiency of QT-1, it was chosen as a photodynamic therapy agent to selectively kill cancer cells from normal cells. Upon light irradiation, an obvious decrease of mitochondrial membrane potential(MMP) and serious change of mitochondrial shape in cells were observed, which corresponded to the efficient inhibition of tumor growth in vivo. This work afforded a promising strategy for the construction of multicolor emission by tuning anti-Kasha behaviors and expanding their application in dualorganelle targeting-based phototheranostics.
基金support by the National Natural Science Foundation of China(22275072)Guangdong Provincial Key laboratory of Luminescence from Molecular Aggregates(2019B030301003)Scientific and Technological Innovation Team of Shaanxi Province(2022TD-36).
文摘Tetraphenylpyrazine(TPP)is a promising heterocycle-based aggregation-induced emission luminogen(AIEgen)which has sparked multiple applications in organic light-emitting diodes,sensors,and biotherapy.However,the utility of it in developing information storage materials is relatively rare.Moreover,TPP is mostly employed as an electronic acceptor in molecular design,while the consideration of it as an electronic donor is attractive in studies which may provide a full understanding of its property to tailor the materials.In this work,we synthesize three TPP-based molecules by decorating it with acrylonitrile and isomeric pyridine units,which show AIE behavior by property inheritance from their parent unit.Interestingly,the effective intramolecular charge transfer takes place from the TPP electronic donor to the acrylonitrile and pyridine electronic acceptor,therefore inducing a remarkable solvatochromic effect as the solvent polarity improves.Moreover,it is revealed that the isomeric effect of the nitrogen atom in the pyridines may pose an influence on the absorption,solvatochromism,and AIE behavior.In addition,the acrylonitrile and pyridine groups are reactive to light and acid-base stimuli with irreversible and reversible responses,respectively.Combined with the high light-harvesting ability of these AIEgens,they show great potential in the stimuli-responsive materials for dual information storage.
基金The authors gratefully acknowledge the Research Foundation of Education Department of Shaanxi Province(23JK0282)fund of Rising Stars of Shaanxi Province(2021KJXX-48)+2 种基金the National Natural Science Foundation of China(52173152 and 21805002)the Scientific and Technological Innovation Team of Shaanxi Province(2022TD-36)the Natural Science Basic Research Program of Shaanxi Province(2024JC-YBQN-0107,2024JC-YBMS-114,and 2024JC-YBQN-0782).
文摘To meet the high requirements of biomedical applications in antimicrobial agents, it is crucial to explore efficient nanoantimicrobialagents with no resistance and good biocompatibility for treating infected wounds. In this study, compositenano-antibiotic TPA-Py@AuNCs⊂BSA nanoparticles (TAB NPs) are prepared using hollow mesoporous Au nanocages (AuNCs)loaded with a photosensitizer (namely TPA-Py) with D-π-A structure showing aggregation-induced emission properties. WhenTPA-Py is encapsulated in the cavity of AuNCs, its fluorescence is suppressed. In the presence of photothermal induction, TPA-Pycan be released from the AuNCs, allowing for the restoration of fluorescence illumination and the specific imaging of Grampositivebacteria. TAB NPs demonstrate outstanding antimicrobial activity against a variety of bacteria, and this multimodalantimicrobial property does not lead to the development of bacterial resistance. In vitro experiments show that TAB NPs couldeliminate bacteria and ablate bacterial biofilm. In vivo experiments show that the synergistic antimicrobial effect of TAB NPs has asignificant positive impact on the treatment of infectedwounds, including rapid antibacterial action, promotion of M2 macrophagepolarization, and enhancement of chronic wound healing. This study provides an effective strategy for developing wide-spectrumnano-antibiotics for the ablation of bacterial biofilms and the treatment of infected wounds.
基金National Natural Science Foundation of China,Grant/Award Numbers:52173152,21805002The Fund of the Rising Stars of Shaanxi Province,Grant/Award Number:2021KJXX-48+5 种基金The Natural Science Basic Research Plan in Shaanxi Province of China,Grant/Award Number:2023-JC-QN-0163Young Talent Fund of University Association for Science and Technology in Shaanxi,China,Grant/Award Numbers:20190610,20210606Research Foundation of Education Department of Shaanxi Province,Grant/Award Number:21JK0487Scientific and Technological Innovation Team of Shaanxi Province,Grant/Award Number:2022TD-36Basic and Applied Basic Research Foundation of Guangdong Province,Grant/Award Number:2020A1515110476College Students’Innovative Entrepreneurial Training Plan Program of Baoji University of Arts and Sciences,Grant/Award Number:S202210721040。
文摘Solar-driven interfacial evaporation is a promising technology for desalination.The photothermal conversion materials are at the core and play a key role in thisfield.Design of photothermal conversion materials based on organic dyes for desalina-tion is still a challenge due to lack of efficient guiding strategy.Herein,a new D(donor)-A(acceptor)type conjugated tetraphenylpyrazine(TPP)luminophore(namely TPP-2IND)was prepared as a photothermal conversion molecule.It exhib-ited a broad absorption spectrum and strongπ–πstacking in the solid state,resulting in efficient sunlight harvesting and boosting nonradiative decay.TPP-2IND powder exhibited high photothermal efficiency upon 660 nm laser irradiation(0.9 W cm^(-2)),and the surface temperature can reach to 200℃.Then,an interfacial heating system based on TPP-2IND is established successfully.The water evaporation rate and the solar-driven water evaporation efficiency were evaluated up to 1.04 kg m^(-2) h^(-1) and 65.8%under 1 sunlight,respectively.Thus,this novel solar-driven heating system shows high potential for desalination and stimulates the development of advanced photothermal conversion materials.
基金National Natural Science Foundation of China,Grant/Award Numbers:52173152,21805002Guangdong Basic and Applied Basic Research Foundation,Grant/Award Number:2020A1515110476+4 种基金Fund of the Rising Stars of Shaanxi Province,Grant/Award Number:2021KJXX-48Natural Science Basic Research Plan in Shaanxi Province of China,Grant/Award Numbers:2019JQ-302,2021JQ-801Research Foundation of Education Department of Shaanxi Province,Grant/Award Number:20JS005Young Talent fund of University Association for Science and Technology in Shaanxi,China,Grant/Award Numbers:20190610,20210606Scientific and Technological Innovation Team of Shaanxi Province,Grant/Award Number:2022TD-36。
文摘Enantioselective recognition and separation are the most important issues in the fields of chemistry,pharmacy,agrochemical,and food science.Here,we developed two optically active diamines showing aggregation-induced emission(AIE)that can discriminate 5 kinds of chiral acids with high enantioselectivity.Especially,a very high fluorescence intensity ratio(IL/ID)of 281 for(±)-Dibenzoyl-D/L-tartaric acid was obtained through the collection of fluorescence change after interaction with chiral AIE-active diamine.By virtue of AIE property and intermolecular acidbase interaction,enantioselective separation was facilely realized by simple filtration of the precipitates formed by chiral AIE luminogen(AIEgen)and one enantiomer in the racemic solution.The chiral HPLC data indicated that the precipitates of AIEgen/chiral acid possessed 82%L-analyte(the enantiomeric excess value was assessed to be 64%ee).Therefore,this method can serve as a simple,convenient,and low-cost tool for chiral detection and separation.
基金supported by the National Natural Science Foundation of China(grant nos.21788102 and 22101028)the Research Grants Council of Hong Kong(grant nos.16304819,16305320,and C6014-20W)+3 种基金the Innovation and Technology Commission(grant no.ITC-CNERC14SC01)the Natural Science Foundation of Guangdong Province(grant no.2019B121205002)the China Postdoctoral Science Foundation(grant no.2021M691414)the Scientific and Technological Innovation Team of Shaanxi Province(grant no.2022TD-36).
文摘Organic reactions in water have attracted great attention due to their advantages such as unique reaction performance and environmental friendliness.Organic reactions as well as polymerizations in aqueous media have been extensively investigated,and so far,there has been a massive amount of reporting about polymerizations in water.However,reports about click polymerization in water have been rare.Herein,click polymerization of activated alkyne and aromatic amine in aqueous media is developed.The“on water”effect facilitates polymerization in aqueous media better than in organic solvents,and its mechanism is deciphered through experimental data and theoretical calculations.Water participates in the reaction and reduces the energy barrier to some extent.Besides,polymerization makes it possible for aromatic amine with low reactivity to be linked.By using this strategy,polymers with high molecular weights can be obtained in high yields(up to 95.4%).They show good thermal stability and high refractivity.They can be photodegraded.The polymers with tetraphenylethylene moieties show aggregation-induced emission and can be used as materials for generating photopatterns and visualizing agents for specific staining of lysosome in living cells.
