Two novel aggregation-induced emission(AIE)-active probes,TPA-H and TPA-2 F,were designed and synthesized based on a triphenylamine(TPA)core.Systematic characterization demonstrated that both probes exhibit excellent ...Two novel aggregation-induced emission(AIE)-active probes,TPA-H and TPA-2 F,were designed and synthesized based on a triphenylamine(TPA)core.Systematic characterization demonstrated that both probes exhibit excellent biocompatibility(cell viability>90%at concentrations up to 50μmol/L)and outstanding LD-targeting speci⁃ficity with minimal colocalization with other organelles such as mitochondria and lysosomes.During early differentia⁃tion of 3 T 3-L 1 adipocytes,both TPA-2 F and TPA-H clearly visualized small and nascent LDs that were difficult to be detected with BODIPY,indicating superior imaging sensitivity compared to the existing fluorescent probes for LDs.Moreover,TPA-2 F demonstrated exceptional photostability,retaining over 90%of its initial fluorescence intensity after 100 continuous laser scanning cycles,significantly outperforming TPA-H.This work not only provides two high-performance LD imaging tools but also highlights the potential of AIE luminogens(AIEgens)in organelle-specific bioimaging,offering promising avenues for early diagnosis and mechanistic research of lipid-related metabolic diseases.展开更多
A multi-stimuli-responsive hydrogel,P(VI-co-MAAC-NE),was successfully constructed by covalently integrating the aggregation-induced emission(AIE)moiety(Z)-N-(4-(1-cyano-2-(4-(diethylamino)phenyl)vinyl)-phenyl)methacry...A multi-stimuli-responsive hydrogel,P(VI-co-MAAC-NE),was successfully constructed by covalently integrating the aggregation-induced emission(AIE)moiety(Z)-N-(4-(1-cyano-2-(4-(diethylamino)phenyl)vinyl)-phenyl)methacrylamide(NE)into a dynamic hydrogen-bonding network composed of 1-vinylimidazole(VI)and methacrylic acid(MAAC)groups.The dense hydrogen-bonding network not only provides enhanced mechanical robustness,but also significantly enhances the AIE effect of NE by restricting its molecular motion.Under various external stimuli,the hydrogen bonds within the hydrogel network undergo reversible dissociation and reformation,thus enabling synergistic modulation of the hydrogel’s mechanical properties and luminescence behavior.Specifically,organic solvents disrupt the hydrogen-bonding network and the aggregation of the AIE moiety NE,resulting in macroscopic swelling and fluorescence quenching of the hydrogel.In strongly acidic conditions,protonation of NE molecules suppresses the intramolecular charge transfer(ICT)process,yielding a blue-shifted emission band accompanied by intense blue fluorescence;in highly alkaline environments,deprotonation of carboxyl groups induces hydrogel swelling and disperses NE aggregates,leading to pronounced fluorescence quenching.Moreover,the system exhibits thermally activated shape-memory behavior:heating above the glass transition temperature(T_(g):ca.62℃)softens the hydrogel to allow programmable reshaping,and subsequent hydrogen bond reformation at ambient conditions locks in the resultant geometries without sacrificing the hydrogel’s fluorescence performance.By capitalizing on these multi-stimuli-responsive characteristics and shape-memory behavior,the potential of hydrogel P(VI-co-MAAC-NE)for advanced information encryption and anti-counterfeiting applications is demonstrated.This work not only provides a versatile material platform for sensing and information storage,but also offers new insights into the design of intelligent soft materials integrating AIE features with dynamically regulated supramolecular network structures.展开更多
The treatment of ammonia nitrogen wastewater(ANW)has garnered significant attention due to the ecology,and even biology is under increasing threat from over discharge ANW.Conventional ANW treatment methods often encou...The treatment of ammonia nitrogen wastewater(ANW)has garnered significant attention due to the ecology,and even biology is under increasing threat from over discharge ANW.Conventional ANW treatment methods often encounter challenges such as complex processes,high costs and secondary pollution.Considerable progress has been made in employing solar-induced evaporators for wastewater treatment.However,there remain notable barriers to transitioning from fundamental research to practical applications,including insufficient evaporation rates and inadequate resistance to biofouling.Herein,we propose a novel evaporator,which comprises a bio-enzyme-treated wood aerogel that serves as water pumping and storage layer,a cost-effective multi-walled carbon nanotubes coated hydrophobic/hydrophilic fibrous nonwoven mat functioning as photothermal evaporation layer,and aggregation-induced emission(AIE)molecules incorporated as anti-biofouling agent.The resultant bioinspired evaporator demonstrates a high evaporation rate of 12.83 kg m^(−2) h^(−1) when treating simulated ANW containing 30 wt%NH4Cl under 1.0 sun of illumination.AIE-doped evaporator exhibits remarkable photodynamic antibacterial activity against mildew and bacteria,ensuring outstanding resistance to biofouling over extended periods of wastewater treatment.When enhanced by natural wind under 1.0 sun irradiation,the evaporator achieves an impressive evaporation rate exceeding 20 kg m^(−2) h^(−1) .This advancement represents a promising and viable approach for the effective removal of ammonia nitrogen wastewater.展开更多
Prostate cancer(PCa)is characterized by high incidence and propensity for easy metastasis,presenting significant challenges in clinical diagnosis and treatment.Tumor microenvironment(TME)-responsive nanomaterials prov...Prostate cancer(PCa)is characterized by high incidence and propensity for easy metastasis,presenting significant challenges in clinical diagnosis and treatment.Tumor microenvironment(TME)-responsive nanomaterials provide a promising prospect for imaging-guided precision therapy.Considering that tumor-derived alkaline phosphatase(ALP)is over-expressed in metastatic PCa,it makes a great chance to develop a theranostics system with ALP responsive in the TME.Herein,an ALP-responsive aggregationinduced emission luminogens(AIEgens)nanoprobe AMNF self-assembly was designed for enhancing the diagnosis and treatment of metastatic PCa.The nanoprobe exhibited self-aggregation in the presence of ALP resulted in aggregation-induced fluorescence,and enhanced accumulation and prolonged retention period at the tumor site.In terms of detection,the fluorescence(FL)/computed tomography(CT)/magnetic resonance(MR)multi-mode imaging effect of nanoprobe was significantly improved post-aggregation,enabling precise diagnosis through the amalgamation of multiple imaging modes.Enhanced CT/MR imaging can achieve assist preoperative tumor diagnosis,and enhanced FL imaging technology can achieve“intraoperative visual navigation”,showing its potential application value in clinical tumor detection and surgical guidance.In terms of treatment,AMNF showed strong absorption in the near infrared region after aggregation,which improved the photothermal treatment effect.Overall,our work developed an effective aggregation-enhanced theranostic strategy for ALP-related cancers.展开更多
Diseases associated with bacterial infection,especially those caused by gram-negative bacteria,have been posing a serious threat to human health.Photodynamic therapy based on aggregation-induced emission(AIE)photosens...Diseases associated with bacterial infection,especially those caused by gram-negative bacteria,have been posing a serious threat to human health.Photodynamic therapy based on aggregation-induced emission(AIE)photosensitizer have recently emerged and provided a promising approach for bacterial discrimination and efficient photodynamic antimicrobial applications.However,they often suffer from the shorter excitation wavelength and lower molar extinction coefficients in the visible region,severely limiting their further applications.Herein,three novel BF_(2)-curcuminoid-based AIE photosensitizers,TBBC,TBC and TBBC-C8,have been rationally designed and successfully developed,in which OCH_(3)-and OC_(8)H_(17)-substituted tetraphenylethene(TPE)groups serve as both electron donor(D)and AIE active moieties,BF_(2)bdk group functions as electron acceptor(A),and styrene(or ethylene)group asπ-bridge in this D-π-A-π-D system,respectively.As expected,these resulting BF_(2)-curcuminoids presented solvent-dependent photophysical properties with large molar extinction coefficients in solutions and excellent AIE properties.Notably,TBBC showed an effective singlet oxygen generation efficiency thanks to the smaller singlet-triplet energy gap(△E_(ST)),and remarkable photostability under green light exposure at 530nm(8.9 mW/cm^(2)).More importantly,TBBC was demonstrated effectiveness in selective staining and photodynamic killing of Escherichia coli(E.coli)in vitro probably due to its optimal molecular size compared with TBC and TBBC-C8.Therefore,TBBC will have great potential as a novel AIE photosensitizer to apply in the discrimination and selective sterilization between Gram-positive and Gram-negative bacteria.展开更多
文摘Two novel aggregation-induced emission(AIE)-active probes,TPA-H and TPA-2 F,were designed and synthesized based on a triphenylamine(TPA)core.Systematic characterization demonstrated that both probes exhibit excellent biocompatibility(cell viability>90%at concentrations up to 50μmol/L)and outstanding LD-targeting speci⁃ficity with minimal colocalization with other organelles such as mitochondria and lysosomes.During early differentia⁃tion of 3 T 3-L 1 adipocytes,both TPA-2 F and TPA-H clearly visualized small and nascent LDs that were difficult to be detected with BODIPY,indicating superior imaging sensitivity compared to the existing fluorescent probes for LDs.Moreover,TPA-2 F demonstrated exceptional photostability,retaining over 90%of its initial fluorescence intensity after 100 continuous laser scanning cycles,significantly outperforming TPA-H.This work not only provides two high-performance LD imaging tools but also highlights the potential of AIE luminogens(AIEgens)in organelle-specific bioimaging,offering promising avenues for early diagnosis and mechanistic research of lipid-related metabolic diseases.
文摘A multi-stimuli-responsive hydrogel,P(VI-co-MAAC-NE),was successfully constructed by covalently integrating the aggregation-induced emission(AIE)moiety(Z)-N-(4-(1-cyano-2-(4-(diethylamino)phenyl)vinyl)-phenyl)methacrylamide(NE)into a dynamic hydrogen-bonding network composed of 1-vinylimidazole(VI)and methacrylic acid(MAAC)groups.The dense hydrogen-bonding network not only provides enhanced mechanical robustness,but also significantly enhances the AIE effect of NE by restricting its molecular motion.Under various external stimuli,the hydrogen bonds within the hydrogel network undergo reversible dissociation and reformation,thus enabling synergistic modulation of the hydrogel’s mechanical properties and luminescence behavior.Specifically,organic solvents disrupt the hydrogen-bonding network and the aggregation of the AIE moiety NE,resulting in macroscopic swelling and fluorescence quenching of the hydrogel.In strongly acidic conditions,protonation of NE molecules suppresses the intramolecular charge transfer(ICT)process,yielding a blue-shifted emission band accompanied by intense blue fluorescence;in highly alkaline environments,deprotonation of carboxyl groups induces hydrogel swelling and disperses NE aggregates,leading to pronounced fluorescence quenching.Moreover,the system exhibits thermally activated shape-memory behavior:heating above the glass transition temperature(T_(g):ca.62℃)softens the hydrogel to allow programmable reshaping,and subsequent hydrogen bond reformation at ambient conditions locks in the resultant geometries without sacrificing the hydrogel’s fluorescence performance.By capitalizing on these multi-stimuli-responsive characteristics and shape-memory behavior,the potential of hydrogel P(VI-co-MAAC-NE)for advanced information encryption and anti-counterfeiting applications is demonstrated.This work not only provides a versatile material platform for sensing and information storage,but also offers new insights into the design of intelligent soft materials integrating AIE features with dynamically regulated supramolecular network structures.
基金supported by the National Natural Science Foundation of China(52203226)the Fundamental Research Funds for the Central Universities(2232023G-06).
文摘The treatment of ammonia nitrogen wastewater(ANW)has garnered significant attention due to the ecology,and even biology is under increasing threat from over discharge ANW.Conventional ANW treatment methods often encounter challenges such as complex processes,high costs and secondary pollution.Considerable progress has been made in employing solar-induced evaporators for wastewater treatment.However,there remain notable barriers to transitioning from fundamental research to practical applications,including insufficient evaporation rates and inadequate resistance to biofouling.Herein,we propose a novel evaporator,which comprises a bio-enzyme-treated wood aerogel that serves as water pumping and storage layer,a cost-effective multi-walled carbon nanotubes coated hydrophobic/hydrophilic fibrous nonwoven mat functioning as photothermal evaporation layer,and aggregation-induced emission(AIE)molecules incorporated as anti-biofouling agent.The resultant bioinspired evaporator demonstrates a high evaporation rate of 12.83 kg m^(−2) h^(−1) when treating simulated ANW containing 30 wt%NH4Cl under 1.0 sun of illumination.AIE-doped evaporator exhibits remarkable photodynamic antibacterial activity against mildew and bacteria,ensuring outstanding resistance to biofouling over extended periods of wastewater treatment.When enhanced by natural wind under 1.0 sun irradiation,the evaporator achieves an impressive evaporation rate exceeding 20 kg m^(−2) h^(−1) .This advancement represents a promising and viable approach for the effective removal of ammonia nitrogen wastewater.
基金supported by Natural Science Foundation of Jilin Province(No.SKL202302002)Key Research and Development project of Jilin Provincial Science and Technology Department(No.20210204142YY)+2 种基金The Science and Technology Development Program of Jilin Province(No.2020122256JC)Beijing Kechuang Medical Development Foundation Fund of China(No.KC2023-JX-0186BQ079)Talent Reserve Program(TRP),the First Hospital of Jilin University(No.JDYY-TRP-2024007)。
文摘Prostate cancer(PCa)is characterized by high incidence and propensity for easy metastasis,presenting significant challenges in clinical diagnosis and treatment.Tumor microenvironment(TME)-responsive nanomaterials provide a promising prospect for imaging-guided precision therapy.Considering that tumor-derived alkaline phosphatase(ALP)is over-expressed in metastatic PCa,it makes a great chance to develop a theranostics system with ALP responsive in the TME.Herein,an ALP-responsive aggregationinduced emission luminogens(AIEgens)nanoprobe AMNF self-assembly was designed for enhancing the diagnosis and treatment of metastatic PCa.The nanoprobe exhibited self-aggregation in the presence of ALP resulted in aggregation-induced fluorescence,and enhanced accumulation and prolonged retention period at the tumor site.In terms of detection,the fluorescence(FL)/computed tomography(CT)/magnetic resonance(MR)multi-mode imaging effect of nanoprobe was significantly improved post-aggregation,enabling precise diagnosis through the amalgamation of multiple imaging modes.Enhanced CT/MR imaging can achieve assist preoperative tumor diagnosis,and enhanced FL imaging technology can achieve“intraoperative visual navigation”,showing its potential application value in clinical tumor detection and surgical guidance.In terms of treatment,AMNF showed strong absorption in the near infrared region after aggregation,which improved the photothermal treatment effect.Overall,our work developed an effective aggregation-enhanced theranostic strategy for ALP-related cancers.
基金National Natural Science Foundation of China(No.32101150)Key Scientific Research Project of Higher Education of Henan Province(No.22A430007)+2 种基金Natural Science Foundation of Henan Province(No.222300420501)the Science and Technology Project of Henan Province(No.242102230119)Innovation and Entrepreneurship Training Program for College students in China(No.202310482001).
文摘Diseases associated with bacterial infection,especially those caused by gram-negative bacteria,have been posing a serious threat to human health.Photodynamic therapy based on aggregation-induced emission(AIE)photosensitizer have recently emerged and provided a promising approach for bacterial discrimination and efficient photodynamic antimicrobial applications.However,they often suffer from the shorter excitation wavelength and lower molar extinction coefficients in the visible region,severely limiting their further applications.Herein,three novel BF_(2)-curcuminoid-based AIE photosensitizers,TBBC,TBC and TBBC-C8,have been rationally designed and successfully developed,in which OCH_(3)-and OC_(8)H_(17)-substituted tetraphenylethene(TPE)groups serve as both electron donor(D)and AIE active moieties,BF_(2)bdk group functions as electron acceptor(A),and styrene(or ethylene)group asπ-bridge in this D-π-A-π-D system,respectively.As expected,these resulting BF_(2)-curcuminoids presented solvent-dependent photophysical properties with large molar extinction coefficients in solutions and excellent AIE properties.Notably,TBBC showed an effective singlet oxygen generation efficiency thanks to the smaller singlet-triplet energy gap(△E_(ST)),and remarkable photostability under green light exposure at 530nm(8.9 mW/cm^(2)).More importantly,TBBC was demonstrated effectiveness in selective staining and photodynamic killing of Escherichia coli(E.coli)in vitro probably due to its optimal molecular size compared with TBC and TBBC-C8.Therefore,TBBC will have great potential as a novel AIE photosensitizer to apply in the discrimination and selective sterilization between Gram-positive and Gram-negative bacteria.
