Recently,the chemiluminescence(CL)induced by carbon nanodots(CDs)has intrigued researchers’extensive interests in various applications due to its special light emission principle.However,the difficulty of synthesizin...Recently,the chemiluminescence(CL)induced by carbon nanodots(CDs)has intrigued researchers’extensive interests in various applications due to its special light emission principle.However,the difficulty of synthesizing chemiluminescent CDs with full-spectrum emission severely hinders the further regulation of the CL emission mechanism.Herein,the multi-color-emissive chemiluminescent CDs are rational designed and further synthesized by regulating the sp2-hybrid core and sp3-hybrid surface from the citrate-ammonia molecular in a single solvothermal reaction.More experimental characterizations and density functional theory calculations reveal that the higher temperature can promote the crosslinking polymerization/carbonization of carbon core and the higher protonation of solvent can determine the core size of final CDs,resulting in the variant CL emission from molecular-,crosslinking-and core-states.Thus,the CL emission of the CDs can be further synthesized by tuning the luminescence chromophores in the formation process via regulating the temperature and solvent,enabling the applications of the CL CDs in illumination and information encryption.This study paves a new technology to understand the luminescence of CDs and affords an industry translational potential over traditional chemiluminescent molecular.展开更多
Advanced antibacterial technologies are needed to counter the rapid emergence of drug-resistant bacteria.Imageguided therapy is one of the most promising strategies for efficiently and accurately curing bacterial infe...Advanced antibacterial technologies are needed to counter the rapid emergence of drug-resistant bacteria.Imageguided therapy is one of the most promising strategies for efficiently and accurately curing bacterial infections.Herein,a chemiluminescence(CL)-dynamic/guided antibacteria(CDGA)with multiple reactive oxygen species(ROS)generation capacity and chemiexcited near-infrared emission has been designed for the precise theranostics of bacterial infection by employing near-infrared emissive carbon nanodots(CDs)and peroxalate as CL fuels.Mechanistically,hydrogen peroxide generated in the bacterial microenvironment can trigger the chemically initiated electron exchange between CDs and energy-riched intermediate originated from the oxidized peroxalate,enabling bacterial induced inflammation imaging.Meanwhile,type Ⅰ/Ⅱ photochemical ROS production and type Ⅲ ultrafast charge transfer from CDs under the self-illumination can inhibit the bacteria proliferation efficiently.The potential clinical utility of CDGA is further demonstrated in bacteria infected mice trauma model.The self-illuminating CDGA exhibits an excellent in vivo imaging quality in early detecting wound infections and internal inflammation caused by bacteria,and further are proven as efficient broad-spectrum antibacterial nanomedicines without drug-resistance,whose sterilizing rate is up to 99.99%.展开更多
基金the National Natural Science Foundation of China(Nos.U2004168,12074348,11974317,12261141661,and 62204223)the China Postdoctoral Science Foundation(No.2022TQ0307)the Natural Science Foundation of Henan Province(Nos.212300410078 and 222102310664)。
文摘Recently,the chemiluminescence(CL)induced by carbon nanodots(CDs)has intrigued researchers’extensive interests in various applications due to its special light emission principle.However,the difficulty of synthesizing chemiluminescent CDs with full-spectrum emission severely hinders the further regulation of the CL emission mechanism.Herein,the multi-color-emissive chemiluminescent CDs are rational designed and further synthesized by regulating the sp2-hybrid core and sp3-hybrid surface from the citrate-ammonia molecular in a single solvothermal reaction.More experimental characterizations and density functional theory calculations reveal that the higher temperature can promote the crosslinking polymerization/carbonization of carbon core and the higher protonation of solvent can determine the core size of final CDs,resulting in the variant CL emission from molecular-,crosslinking-and core-states.Thus,the CL emission of the CDs can be further synthesized by tuning the luminescence chromophores in the formation process via regulating the temperature and solvent,enabling the applications of the CL CDs in illumination and information encryption.This study paves a new technology to understand the luminescence of CDs and affords an industry translational potential over traditional chemiluminescent molecular.
基金the support of the National Natural Science Foundation of China(U2004168,12074348 and 11974317)the Natural Science Foundation of Henan Province(212300410078).
文摘Advanced antibacterial technologies are needed to counter the rapid emergence of drug-resistant bacteria.Imageguided therapy is one of the most promising strategies for efficiently and accurately curing bacterial infections.Herein,a chemiluminescence(CL)-dynamic/guided antibacteria(CDGA)with multiple reactive oxygen species(ROS)generation capacity and chemiexcited near-infrared emission has been designed for the precise theranostics of bacterial infection by employing near-infrared emissive carbon nanodots(CDs)and peroxalate as CL fuels.Mechanistically,hydrogen peroxide generated in the bacterial microenvironment can trigger the chemically initiated electron exchange between CDs and energy-riched intermediate originated from the oxidized peroxalate,enabling bacterial induced inflammation imaging.Meanwhile,type Ⅰ/Ⅱ photochemical ROS production and type Ⅲ ultrafast charge transfer from CDs under the self-illumination can inhibit the bacteria proliferation efficiently.The potential clinical utility of CDGA is further demonstrated in bacteria infected mice trauma model.The self-illuminating CDGA exhibits an excellent in vivo imaging quality in early detecting wound infections and internal inflammation caused by bacteria,and further are proven as efficient broad-spectrum antibacterial nanomedicines without drug-resistance,whose sterilizing rate is up to 99.99%.