Owing to their high significance in fundamental study and diverse applications,stimuli-responsive and fluorescent polymers,particularly those with cluster-triggered emission(CTE)featured by non-conjugated chromophores...Owing to their high significance in fundamental study and diverse applications,stimuli-responsive and fluorescent polymers,particularly those with cluster-triggered emission(CTE)featured by non-conjugated chromophores,have drawn tremendous attention in recent years.In this work,fluorescent and multi-responsive polysiloxane(FRPS)was synthesized by hydrolytic condensation polymerization of 3-aminopropyl methyl diethoxysilane(APMS)with 3-(N-isopropyl propionamide)iminopropyl methyl diethoxysilane(APMS-NIP),which was formed in situ through aza-Michael addition between APMS and N-isopropyl acrylamide.FRPS was not only highly sensitive to temperature,pH and CO_(2) in water,but also showed an enhanced and stimuli-adjustable fluorescence emission.The effects of monomer feeding,pH and CO_(2) on its lower critical solution temperature and fluorescent property were investigated.FRPS fluorescence emission was ascribed to CTE mechanism.In addition,FRPS was shown to be highly potential as physiological indicator for cell imaging,and for controlled release and trace detection of doxorubicin.This study provides therefore a type of stimuli-responsive and fluorescent material for potential applications in biomedical fields,and it is also of great significance for understanding of the fluorescence mechanism of polysiloxane-based stimuli-responsive polymers.展开更多
Ultralong organic phosphorescence(UOP)materials have garnered significant interest for applications in advanced optical recording and information encryption.However,it remains a formidable challenge achieving manipula...Ultralong organic phosphorescence(UOP)materials have garnered significant interest for applications in advanced optical recording and information encryption.However,it remains a formidable challenge achieving manipulated phosphorescence due to the limited color channels and poorly populated triplet energy levels.Herein,we report a novel multiresponsive organic phosphorescence material,in which the phosphorescence color can be dynamically tuned with stimuli such as radiation duration,concentration,excitation wavelength,time,and temperature.The material is based on the confined 7H-benzo[c]carbazole(BCz)molecules in the polymermatrix,which is achieved through the size-dependent cluster-triggered emission(CTE)mechanism.The BCz molecules form isolated molecules and different-sized clusters in the matrix,resulting in multiple luminescent centers with different energy levels and phosphorescence lifetimes.Throughmatrix confinement effects,the activation states of the monomers and multiple clusters could be precisely modulated,resulting in temperature-controlled tunable orange-to-green variations.Furthermore,the multiresponsive properties of the material have been used in both civil and military applications through sophisticated mathematical modeling.This work potentially proposes a guiding strategy for the development of multiresponsive UOP materials based on CTE molecules.展开更多
基金This work was financially supported by Nature Science Foundation of Shandong Province,China(Nos.ZR2021MB112 and ZR2022MB051)Science and Technology Bureau of Jinan City(No.2021GXRC105)+1 种基金Postdoctoral Science Foundation of China(No.2022M712343)as well as by Basic and Applied Basic Research Foundation(No.2020A1515110374)of Guangdong Province,China.
文摘Owing to their high significance in fundamental study and diverse applications,stimuli-responsive and fluorescent polymers,particularly those with cluster-triggered emission(CTE)featured by non-conjugated chromophores,have drawn tremendous attention in recent years.In this work,fluorescent and multi-responsive polysiloxane(FRPS)was synthesized by hydrolytic condensation polymerization of 3-aminopropyl methyl diethoxysilane(APMS)with 3-(N-isopropyl propionamide)iminopropyl methyl diethoxysilane(APMS-NIP),which was formed in situ through aza-Michael addition between APMS and N-isopropyl acrylamide.FRPS was not only highly sensitive to temperature,pH and CO_(2) in water,but also showed an enhanced and stimuli-adjustable fluorescence emission.The effects of monomer feeding,pH and CO_(2) on its lower critical solution temperature and fluorescent property were investigated.FRPS fluorescence emission was ascribed to CTE mechanism.In addition,FRPS was shown to be highly potential as physiological indicator for cell imaging,and for controlled release and trace detection of doxorubicin.This study provides therefore a type of stimuli-responsive and fluorescent material for potential applications in biomedical fields,and it is also of great significance for understanding of the fluorescence mechanism of polysiloxane-based stimuli-responsive polymers.
基金supported by the National Natural Science Foundation of China(NSFC)(U2241236,1220041913,52473253)the National Key Research and Development Program of China(2022ZDZX0007)+2 种基金Young Elite Scientists Sponsorship Program by CAST(2022QNRC001)Yunnan Major Scientific and Technological Projects(202402AB080011)the Science Fund of Shandong Laboratory of Advanced Materials and Green Manufacturing at Yantai(AMGM2024F15).
文摘Ultralong organic phosphorescence(UOP)materials have garnered significant interest for applications in advanced optical recording and information encryption.However,it remains a formidable challenge achieving manipulated phosphorescence due to the limited color channels and poorly populated triplet energy levels.Herein,we report a novel multiresponsive organic phosphorescence material,in which the phosphorescence color can be dynamically tuned with stimuli such as radiation duration,concentration,excitation wavelength,time,and temperature.The material is based on the confined 7H-benzo[c]carbazole(BCz)molecules in the polymermatrix,which is achieved through the size-dependent cluster-triggered emission(CTE)mechanism.The BCz molecules form isolated molecules and different-sized clusters in the matrix,resulting in multiple luminescent centers with different energy levels and phosphorescence lifetimes.Throughmatrix confinement effects,the activation states of the monomers and multiple clusters could be precisely modulated,resulting in temperature-controlled tunable orange-to-green variations.Furthermore,the multiresponsive properties of the material have been used in both civil and military applications through sophisticated mathematical modeling.This work potentially proposes a guiding strategy for the development of multiresponsive UOP materials based on CTE molecules.
