Near-infrared(NIR)small molecular organic dyes as photothermal agents for cancer photothermal therapy(PTT)have attracted considerable research attention.Herein,two donor-acceptor-donor(D-A-D)structured NIR dyes,BBTT a...Near-infrared(NIR)small molecular organic dyes as photothermal agents for cancer photothermal therapy(PTT)have attracted considerable research attention.Herein,two donor-acceptor-donor(D-A-D)structured NIR dyes,BBTT and SeBTT,are rationally designed,where the only difference is one heteroatom within the acceptor unit varying from sulfur to selenium(Se).More importantly,SeBTT NPs exhibit stronger NIR absorbance and higher photothermal conversion efficiency(PTCE≈65.3%).In vivo experiments illustrate that SeBTT NPs can be utilized as a high contrast photoacoustic imaging(PAI)agent,and succeed in tumor suppression without noticeable damage to main organs under NIR photoirradiation.This study presents an effective molecular heteroatom surgery strategy to regulate the photothermal properties of NIR small molecules for enhanced PAI and PTT.展开更多
A novel versatile photocatalyst, FDU-PdPcS, was prepared by immobilizing palladium phthalocyaninesulfonate （PdPcS） onto the FDU-15 mesopolymer via multi-step chemical modification processes involving chloromethylati...A novel versatile photocatalyst, FDU-PdPcS, was prepared by immobilizing palladium phthalocyaninesulfonate （PdPcS） onto the FDU-15 mesopolymer via multi-step chemical modification processes involving chloromethylation of the FDU-15 mesopolymer first with chloromethyl methyl ether, a subsequent amination reaction with ethylenediamine, and finally modification with palladium phthalocyaninesulfonate via ionic interaction. The obtained FDU-PdPcS photocatalyst was characterized by the X-ray diffraction （XRD）, UV-Vis spectrosopy and inductively coupled plasma （ICP） techniques. This photocatalyst not only affords a high dispersion of monomeric PdPcS molecules, which may further be stabilized by the π-electron of benzene rings of FDU-15, but also provides a number of diamino groups inside the mesopores, which could be advantageous for the photodegradation of phenolic pollutants. In photodegradation studies of phenolic pollutants, the FDU-PdPcS catalyst exhibited excellent visible light photocatalytic activity and reusability. The photodegradation products of phenol and bisphenol A were investigated by the gas chromatoghraphy-mass spectrometry （GC-MS） technique. The results showed that the photodegradation products were composed of carboxylic acids and CO2. Isopropanol, sodium azide and benzoquinone were used as hydroxyl radical （OH.）, singlet oxygen （1O2） and superoxide radical （O2.-） scavengers, respectively. The results suggested that 1O2 and O2. were the prominent active species during the photodegradation process. A possible mechanism for the photodegradation of phenol was also discussed.展开更多
Chlorite(ClO_(2)^(−)or COI)is used to establish the advanced reduction and oxidation process(AROP).The iron/biochar-based particles(iron-based hydrothermal carbon with hinge-like structure,FebHCs,20 mg/L)can be utiliz...Chlorite(ClO_(2)^(−)or COI)is used to establish the advanced reduction and oxidation process(AROP).The iron/biochar-based particles(iron-based hydrothermal carbon with hinge-like structure,FebHCs,20 mg/L)can be utilized to activate COI(2 mmol/L)to present selective oxidation in removing triphenylmethane derivatives(15 min,90%).The protonation(H+at~102μmol/L level)played a huge role(k-2nd=0.136c-H+−0.014(R^(2)-adj=0.986),and rapp=−0.0876/c-H++1.017(R^(2)-adj=0.996))to boost the generation of the active species(e.g.,high-valent iron oxidizing species(HVI=O)and chlorine dioxide(ClO_(2))).The protonation-coupled electron transfer promoted Fe-substances in Feb/HCs activating COI(the calculated kobs ranging from 0.066−0.285 min^(−1)).The form of ClO_(2) mainly attributed to proton-coupled electron transfer(1e/1H+).The HVI=O was generated from the electron transfer within the coordination complex.Moreover,carbon particles in FebHCs serve as the bridge for electron transfer.The above roles contribute to the fracture and formation of coordination-induced bonds between Lx-FeII/III and ClO_(2)^(−)at phase interface to form AROP.The ultrasonic(US)cavitation enhanced the mass transfer of active species in bulk solution,and the HVI=O and ClO_(2) attack unsaturated central carbon atoms of triphenylmethane derivatives to initiate selective removal.Furthermore,the scale-up experiment with continuous flow(k values of approximately 0.2 min^(−1),COD removal efficiency of approximately 80%)and the reactor with COMSOL simulation have also proved the applicability of the system.The study offers a novel AROP and new insights into correspondingly heterogeneous interface activation mechanisms.展开更多
基金supported by Natural Science Foundation of Jiangsu Province(No.BK20200092)National Natural Science Foundation of China(No.52072172)Six Talent Peak Innovation Team in Jiangsu Province(No.TD-SWYY-009)。
文摘Near-infrared(NIR)small molecular organic dyes as photothermal agents for cancer photothermal therapy(PTT)have attracted considerable research attention.Herein,two donor-acceptor-donor(D-A-D)structured NIR dyes,BBTT and SeBTT,are rationally designed,where the only difference is one heteroatom within the acceptor unit varying from sulfur to selenium(Se).More importantly,SeBTT NPs exhibit stronger NIR absorbance and higher photothermal conversion efficiency(PTCE≈65.3%).In vivo experiments illustrate that SeBTT NPs can be utilized as a high contrast photoacoustic imaging(PAI)agent,and succeed in tumor suppression without noticeable damage to main organs under NIR photoirradiation.This study presents an effective molecular heteroatom surgery strategy to regulate the photothermal properties of NIR small molecules for enhanced PAI and PTT.
基金supported by the National Natural Science Foundation of China (No. 21143009, 20925310)the Natural Science Foundation of Jiangsu Education Departmen (No. 09KJB150013)+1 种基金the Jiangsu Fundament of "Qilan Project", Jiangsu Provincial Key Laboratory of Coastal Wetland Bioresources and Environmental Protection (No.JLCBE07011)the Research projects of Yancheng Science and Technology Bureau (No. YK2009028)
文摘A novel versatile photocatalyst, FDU-PdPcS, was prepared by immobilizing palladium phthalocyaninesulfonate （PdPcS） onto the FDU-15 mesopolymer via multi-step chemical modification processes involving chloromethylation of the FDU-15 mesopolymer first with chloromethyl methyl ether, a subsequent amination reaction with ethylenediamine, and finally modification with palladium phthalocyaninesulfonate via ionic interaction. The obtained FDU-PdPcS photocatalyst was characterized by the X-ray diffraction （XRD）, UV-Vis spectrosopy and inductively coupled plasma （ICP） techniques. This photocatalyst not only affords a high dispersion of monomeric PdPcS molecules, which may further be stabilized by the π-electron of benzene rings of FDU-15, but also provides a number of diamino groups inside the mesopores, which could be advantageous for the photodegradation of phenolic pollutants. In photodegradation studies of phenolic pollutants, the FDU-PdPcS catalyst exhibited excellent visible light photocatalytic activity and reusability. The photodegradation products of phenol and bisphenol A were investigated by the gas chromatoghraphy-mass spectrometry （GC-MS） technique. The results showed that the photodegradation products were composed of carboxylic acids and CO2. Isopropanol, sodium azide and benzoquinone were used as hydroxyl radical （OH.）, singlet oxygen （1O2） and superoxide radical （O2.-） scavengers, respectively. The results suggested that 1O2 and O2. were the prominent active species during the photodegradation process. A possible mechanism for the photodegradation of phenol was also discussed.
基金supported by the Natural Science foundation of the Jiangsu Higher Education Institutions(No.24KJB610019)the Scientific Research Foundation of Yancheng Teachers University(No.204060047)the Horizontal Topic Research“Developing the environmental remediation technology by acoustic catalysis”(No.203060199).
文摘Chlorite(ClO_(2)^(−)or COI)is used to establish the advanced reduction and oxidation process(AROP).The iron/biochar-based particles(iron-based hydrothermal carbon with hinge-like structure,FebHCs,20 mg/L)can be utilized to activate COI(2 mmol/L)to present selective oxidation in removing triphenylmethane derivatives(15 min,90%).The protonation(H+at~102μmol/L level)played a huge role(k-2nd=0.136c-H+−0.014(R^(2)-adj=0.986),and rapp=−0.0876/c-H++1.017(R^(2)-adj=0.996))to boost the generation of the active species(e.g.,high-valent iron oxidizing species(HVI=O)and chlorine dioxide(ClO_(2))).The protonation-coupled electron transfer promoted Fe-substances in Feb/HCs activating COI(the calculated kobs ranging from 0.066−0.285 min^(−1)).The form of ClO_(2) mainly attributed to proton-coupled electron transfer(1e/1H+).The HVI=O was generated from the electron transfer within the coordination complex.Moreover,carbon particles in FebHCs serve as the bridge for electron transfer.The above roles contribute to the fracture and formation of coordination-induced bonds between Lx-FeII/III and ClO_(2)^(−)at phase interface to form AROP.The ultrasonic(US)cavitation enhanced the mass transfer of active species in bulk solution,and the HVI=O and ClO_(2) attack unsaturated central carbon atoms of triphenylmethane derivatives to initiate selective removal.Furthermore,the scale-up experiment with continuous flow(k values of approximately 0.2 min^(−1),COD removal efficiency of approximately 80%)and the reactor with COMSOL simulation have also proved the applicability of the system.The study offers a novel AROP and new insights into correspondingly heterogeneous interface activation mechanisms.
