Purpose:To design interdialytic and daily weight gain graphs for patients on maintenance haemodialysis and to evaluate their effect on patient adherence to restricted fluid intake.Methods:Forty-five patients on mainte...Purpose:To design interdialytic and daily weight gain graphs for patients on maintenance haemodialysis and to evaluate their effect on patient adherence to restricted fluid intake.Methods:Forty-five patients on maintenance haemodialysis were recruited from August to October 2012.The graphs were applied for 12 weeks based on Bandura’s self-efficacy theory.Adherence to restricted fluid intake,dialysis adequacy,and satisfaction were compared before and after the graphs were applied.Results:Adherence to restricted fluid intake increased from 53.3%to 91.1%;the mean rate of urea clearance(Kt/V)decreased from 1.197 to 1.311,and the qualified rate increased from 42.5%to 70%.The rate of adherence was 86.77%;acceptance and satisfaction rates were 100%.Conclusion:It is acceptable to apply the graphs clinically for subsequent effective improvement of adherence to restricted fluid intake,promoting dialysis adequacy,and increasing patient satisfaction.Therefore,clinical application of the graphs is worthwhile.展开更多
Tuberculosis(TB)is an infectious disease caused by Mycobacterium tuberculosis.Although the diagnostic technology of pulmonary tuberculosis(PTB)has advanced,accurate and differential diagnoses of PTB are still challeng...Tuberculosis(TB)is an infectious disease caused by Mycobacterium tuberculosis.Although the diagnostic technology of pulmonary tuberculosis(PTB)has advanced,accurate and differential diagnoses of PTB are still challenging.In recent years,the rapid development of artificial intelligence(AI)and its wide application in the medical field have provided new opportunities for diagnosing and treating TB and PTB.The machine learning model of AI has not only helped physicians improve diagnostic accuracy,but also enabled them to make early preventive diagnoses for individuals at increased risk of infection.Furthermore,AI can guide physicians to formulate targeted treatment strategies for PTB patients with different conditions.展开更多
High-efficiency and low-cost near-infrared(NIR)emitting quantum dots(QDs)are highly desirable for next-generation intrinsically flexible NIR light sources.Halide passivation is commonly employed to passivate surface t...High-efficiency and low-cost near-infrared(NIR)emitting quantum dots(QDs)are highly desirable for next-generation intrinsically flexible NIR light sources.Halide passivation is commonly employed to passivate surface traps to obtain high-quality NIRemitting PbS QDs,but this procedure requires high temperature and inert atmospheres.Here we develop a facile roomtemperature halide passivation method for highly efficient NIR-emitting PbS QDs by employing crown ethers as a unique auxiliary additive.Experimental and theoretical investigations reveal that the formation of K^(+)-crown ethers complex effectively facilitates the dissociation of KCl in toluene and releases more Cl^(−)ions for extraordinary halide passivation at room temperature and in the air,thus improving the photoluminescence quantum yield from 24%to 35%in solution and further to 44%in blend films.The well-passivated PbS QD films are integrated with red organic light-emitting diodes(OLEDs)and the resulting QDOLEDs exhibit high-performance NIR emission centered at 887 nm,a high external quantum efficiency of 5.2%at a radiance of 10 W·sr^(−1)·m^(−2),superior operational stability with long lifetime T90 of 188 h at the current density of 25 mA·cm^(−2).We also construct a large-area NIR QD-OLED(5 cm×5 cm)with desirable uniform emission.This work opens a new avenue to achieve robust large-area NIR planar light sources for broad applications.展开更多
Protein protected gold nanoclusters have outstanding physical and chemical properties that make them excellent scaffolds for the construction of novel chemical and biological probes. In this study, a simple one-pot sy...Protein protected gold nanoclusters have outstanding physical and chemical properties that make them excellent scaffolds for the construction of novel chemical and biological probes. In this study, a simple one-pot synthesis method was proposed for the preparation of fluorescent probes based on ovalbumin-stabilized gold nanoclusters. This strategy allowed the generation of water-soluble gold nanoclusters within 5 min. The as-prepared fluorescent probe exhibited a red fluorescence emission at 625 nm, and good thermostability. The fluorescent probe was applied to measure glucose concentrations based on the hydrogen peroxide-induced fluorescence quenching principle, and showed favorable biocompatibility, high sensitivity and good selectivity. As a result of the advantageous properties and performance of this fluorescent probe, the present assay allowed for the selective determination of glucose in the range of 5.0×10-6 to 10.0×10-3 mol/L with a detection limit of 1.0×10?6 mol/L. Moreover, the glucose content in urinary samples was analyzed using the constructed fluorescent probe: this indicated the potential of the fluorescent gold nanoclusters for applications in biological and clinical diagnosis and therapy.展开更多
Gold nanoclusters were rapid synthesized within 3 min at 120 ℃ by using papaya juice as a capping and reducing agent(P-AuNCs). The properties of the fluorescent probe were characterized by fluorescent spectroscopy, U...Gold nanoclusters were rapid synthesized within 3 min at 120 ℃ by using papaya juice as a capping and reducing agent(P-AuNCs). The properties of the fluorescent probe were characterized by fluorescent spectroscopy, UV-vis spectroscopy, dynamic light scattering and transmission electron microscope.Based on the surface electron density increase-induced fluorescence enhancing principle, a high selective method for detection of L-lysine was developed with the as-prepared P-AuNCs coupling the fluorescence emission at 440 nm. The fluorescent probe showed high stability and good biocompatibility. Its fluorescence intensity was found to be linearly dependent on the L-lysine concentration in the range of 10.0μmol/L to 1000.0 μmol/L(R^2=0.969) with a limit of detection of 6.0μmol/L. Furthermore, the PAuNCs based approach was applied for monitoring the urine L-lysine contents, demonstrating great potential of fluorescent probes in real samples analysis.展开更多
The temperature monitoring of treated cancer cells is critical in photothermal therapy.Current methods of detecting intracellular temperatures have low accuracy and poor spatial resolution,which limits their applicati...The temperature monitoring of treated cancer cells is critical in photothermal therapy.Current methods of detecting intracellular temperatures have low accuracy and poor spatial resolution,which limits their application to photothermal therapy.Herein,a strategy for targeted recognition and selective capture of MCF-7 breast cancer cells based on fluorescent polymer poly(N-isopropylacrylamide-benzoxadiazole-2-vinyl-4,4-dimethyl azlactone,PNMV)and modified gold nanobipyramids(Au NBPs-PNMV)was developed for temperature sensing during photothermal therapy.A mucin-1 protein aptamer(Apt)was applied to selectively target mucin-1 protein overexpressed on the surfaces of the MCF-7 cells,which can reduce interference by affinity interaction between the Apt and proteins.During photothermal therapy,the significant Au NBPs photothermal effect increases the fluorescence intensity of PNMV with temperature.Irradiation of MCF-7 cells cultured with Au NBPs-PNMV@Apt by an 808 nm laser increases the temperature of the system,while the cells can be inactivated because of the remarkable Au NBPs-PNMV@Apt photothermal effect.The results indicate that variation in the fluorescence of Au NBPs-PNMV@Apt can be applied as thermometers to monitor the intracellular effect of photothermal therapy.展开更多
Pursuing purely organic materials with high-efficiency near-infrared(NIR) emissions is fundamentally limited by the large nonradiative decay rates(k_(nr)) governed by the energy gap law. To date, reported endeavors to...Pursuing purely organic materials with high-efficiency near-infrared(NIR) emissions is fundamentally limited by the large nonradiative decay rates(k_(nr)) governed by the energy gap law. To date, reported endeavors to decelerate k_(nr) are mainly focused on reducing the electron-vibration coupling with the electronic nonadiabatic coupling assumed as a constant. Here, we demonstrated a feasible and innovative strategy by employing intermolecular charge-transfer(CT) aggregates(CTA) to realize high-efficiency NIR emissions via nonadiabatic coupling suppression. The formation of CTA engenders intermolecular CT in the excited states;thereby, not only reducing the electronic nonadiabatic coupling and contributing to small k_(nr) for high-efficiency NIR photoluminescence, but also stabilizing excited-state energies and achieving thermally activated delayed fluorescence for highefficiency NIR electroluminescence. This work provides new insights into aggregates and opens a new avenue for organic materials to overcome the energy gap law and achieve high-efficiency NIR emissions.展开更多
Ovalbumin-stabilized gold nanoclusters (OVA@AuNCs) were prepared with ascorbic acid as a reducing agent. This strategy could realize the synthesis of water-soluble OVA@AuNCs within 20 min. The asprepared fluorescent...Ovalbumin-stabilized gold nanoclusters (OVA@AuNCs) were prepared with ascorbic acid as a reducing agent. This strategy could realize the synthesis of water-soluble OVA@AuNCs within 20 min. The asprepared fluorescent probe showed a red fluorescence emission at 630 nm. Moreover, the properties of the OVA@AuNCs were characterized by transmission electron microscope, dynamic light scattering, ultraviolet-visible spectroscopy, fluorescent spectroscopy. Based on the surface electron density decrease-induced fluorescence quenching mechanism, the OVA@AuNCs provided high sensitivity and selectivity for sensing copper ions. A good linear relationship was obtained between the fluorescence intensity of OVA@AuNCs and the concentration of copper ions in the range of 5.0-100.0pumol/L (R2z0.999) with a detection limit of 640 nmol/L. Furthermore, the rat serum copper contents were determined by using the OVA@AuNCs based assay, indicating great potential of fluorescent probes for application in biological and clinical analysis.展开更多
With _D-proline as the reducing and capping agent, fluorescent gold nanoclusters were rapidly prepared(_D-Pro@AuNCs) within 10 min at 100℃. In the present of gold nanoparticles, the fluorescence of _DPro@AuNCs was re...With _D-proline as the reducing and capping agent, fluorescent gold nanoclusters were rapidly prepared(_D-Pro@AuNCs) within 10 min at 100℃. In the present of gold nanoparticles, the fluorescence of _DPro@AuNCs was remarkably quenched. Interestingly, based on the electrostatic interaction between anticancer drug Raltitrexed and gold nanoparticles induced fluorescence "turn-on" principle, a high selective assay for detection of Raltitrexed was established with the probe associating the fluorescence emission at 435 nm. The fluorescence intensity of _D-Pro@AuNCs linearly correlated with the concentration of Raltitrexed in the range from 5.0 mmol/L to 40.0 mmol/L(R^2= 0.999) and the limit of detection was 1.9 mmol/L. Further, after Raltitrexed was abdominal injected in rats, a metabolic approach was constructed with the prepared fluorescent probe. It showed great potential of AuNCs-based sensing probes for application in analysis of serum anticancer drugs.展开更多
A new open-tubular capillary electrochromatography (OT-CEC) method for analysis of β-lactam antibiotics has been developed with unique block co-polymer coating. To obtain the highly ordered block polymer chains, reve...A new open-tubular capillary electrochromatography (OT-CEC) method for analysis of β-lactam antibiotics has been developed with unique block co-polymer coating. To obtain the highly ordered block polymer chains, reversible addition fragmentation chain transfer radical polymerization method was used to synthesize poly (maleic anhydride-styrene-N-isopropylacrylamide). The prepared block copolymer coating was characterized with NMR, fourier transform infrared spectroscopy and scanning electron microscope. Several key separation factors of OT-CEC, which including polymer amount,stability of the coating, temperature, species of organic additives, buffer pH and concentration, were investigated in detail. Our results indicated that the separation efficiency was improved greatly with the coating capillary and the three test analytes could be baseline separated. Then, the separation mechanism was briefly explored. Moreover, the proposed OT-CEC method displayed promising quantitative analysis property of the three test analytes with good linearity (R2>0.99), repeatability (relative standard deviations <0.9%) and high recovery (95.4%-106.2%). Further, the assay was applied in monitoring the three test β-lactam antibiotics (cephradine, cephalexin and amoxicillin) in serum samples, providing a useful platform for construction of novel polymer coatings in OT-CEC system and for analysis of drugs in real bio-samples.展开更多
Immobilization of enzymes onto carriers is a rapidly growing research area aimed at increasing the stability,reusability and enzymolysis efficiency of free enzymes.In this work,the role of phaseseparation and a pH-res...Immobilization of enzymes onto carriers is a rapidly growing research area aimed at increasing the stability,reusability and enzymolysis efficiency of free enzymes.In this work,the role of phaseseparation and a pH-responsive"hairy"brush,which greatly affected the topography of porous polymer membrane enzyme reactors(PMER),was explored.The porous polymer membrane was fabricated by phase-separation of poly(styrene-co-maleic anhydride-acrylic acid)and poly(styrene-ethylene glycol).Notably,the topography and pores size of the PMER could be controlled by phase-separation and a pHresponsive"hairy"brush.For evaluating the enzymolysis efficiency of D-amino acid oxidase(DAAO)immobilized carrier(DAAO@PMER),a chiral ligand exchange capillary electrophoresis method was developed with D-methionine as the substrate.The DAAO@PMER showed good reusability and stability after five continuous runs.Notably,comparing with free DAAO in solution,the DAAO@PMER exhibited a17.7-folds increase in catalytic velocity,which was attributed to its tailorable topography and pHresponsive property.The poly(acrylic acid)moiety of poly(styrene-co-maleic anhydride-acrylic acid)as the pH-responsive"hairy"brush generated topography changing domains upon adjusting the buffer pH,which enable the enzymolysis efficiency of DAAO@PMER to be tuned based upon the well-defined architectures of the PMER.This approach demonstrated that the topographical changes formed by phaseseparation and the pH-responsive"hairy"brush indeed made the proposed porous polymer membrane as suitable supports for enzyme immobilization and fitting for enzymolysis applications,achieving high catalytic performance.展开更多
Herein, a novel probe based on poly(N,N′-methylenebisacylamide) protected Au NPs(PDMAM-Au NPs) was developed for determination of silver ions. The thiol-terminated PDMAM was synthesized by the reversible addition fra...Herein, a novel probe based on poly(N,N′-methylenebisacylamide) protected Au NPs(PDMAM-Au NPs) was developed for determination of silver ions. The thiol-terminated PDMAM was synthesized by the reversible addition fragmentation chain transfer radical polymerization. Then, the PDMAM-Au NPs were prepared by a simple, one-pot and green process. It has been observed that existence of the silver ions evoked a small red-shift to the emission peak of PDMAM-Au NPs and an obvious increase in UV absorption. The detection limit of the present method for silver ions was 0.5 ?mol/L, with a linear range of 1.0–1000 ?mol/L. Moreover, the possible mechanism for enhanced UV absorption intensity with enlarged diameter of PDMAM-Au NPs was explored and discussed briefly. The results demonstrated that silver ions could be detected by the PDMAM-Au NPs based colorimetric assays, further opening up new ways for the visualization and quantification of silver ions involved in our daily life.展开更多
The operational stability of organic(opto)electronic devices largely depends on the intrinsic stability of organic materials on service.For organic light-emitting diode(OLED)materials,a key parameter of their intrinsi...The operational stability of organic(opto)electronic devices largely depends on the intrinsic stability of organic materials on service.For organic light-emitting diode(OLED)materials,a key parameter of their intrinsic stability is the bond-dissociation energy of the most fragile bond(BDE_(f)).Although rarely involved,many OLED molecules have the lowest BDE_(f) in anionic states[BDE_(f)(−)∼1.6–2.5 eV],which could be a fatal short-slab for device stability.Herein,we separated BDE_(f)(−)from other parameters and confirmed the clear relationship between BDE_(f)(−),intrinsic material stability and device lifetime.Based on thermodynamic principles,we developed a general and effective strategy to greatly improve BDE_(f)(−)by introducing a negative charge manager within the molecule.The manager must combine an electron-withdrawing group(EWG)with a delocalizing structure,so that it can firmly confine the negative charge and hinder the charge redistribution toward fragile bonds.Consequently,the use of this manager can substantially promote BDE_(f)(−)by∼1 eV for various fragile bonds and outperform the effect reported from solely employing EWGs or delocalizing structures.This effect was verified in typical phosphine-oxide and carbazole derivatives and backed up by newly designed molecules with multiple fragile bonds.This strategy provides a new way to transform vulnerable building blocks into robust organic(opto)electronic materials and devices.展开更多
文摘Purpose:To design interdialytic and daily weight gain graphs for patients on maintenance haemodialysis and to evaluate their effect on patient adherence to restricted fluid intake.Methods:Forty-five patients on maintenance haemodialysis were recruited from August to October 2012.The graphs were applied for 12 weeks based on Bandura’s self-efficacy theory.Adherence to restricted fluid intake,dialysis adequacy,and satisfaction were compared before and after the graphs were applied.Results:Adherence to restricted fluid intake increased from 53.3%to 91.1%;the mean rate of urea clearance(Kt/V)decreased from 1.197 to 1.311,and the qualified rate increased from 42.5%to 70%.The rate of adherence was 86.77%;acceptance and satisfaction rates were 100%.Conclusion:It is acceptable to apply the graphs clinically for subsequent effective improvement of adherence to restricted fluid intake,promoting dialysis adequacy,and increasing patient satisfaction.Therefore,clinical application of the graphs is worthwhile.
基金supported by the Special Research on Health and Epidemic Prevention(No.22FYFH13).
文摘Tuberculosis(TB)is an infectious disease caused by Mycobacterium tuberculosis.Although the diagnostic technology of pulmonary tuberculosis(PTB)has advanced,accurate and differential diagnoses of PTB are still challenging.In recent years,the rapid development of artificial intelligence(AI)and its wide application in the medical field have provided new opportunities for diagnosing and treating TB and PTB.The machine learning model of AI has not only helped physicians improve diagnostic accuracy,but also enabled them to make early preventive diagnoses for individuals at increased risk of infection.Furthermore,AI can guide physicians to formulate targeted treatment strategies for PTB patients with different conditions.
基金the National Key Research and Development Program of China(No.2020YFA0715000)the National Natural Science Foundation of China(No.51773109).
文摘High-efficiency and low-cost near-infrared(NIR)emitting quantum dots(QDs)are highly desirable for next-generation intrinsically flexible NIR light sources.Halide passivation is commonly employed to passivate surface traps to obtain high-quality NIRemitting PbS QDs,but this procedure requires high temperature and inert atmospheres.Here we develop a facile roomtemperature halide passivation method for highly efficient NIR-emitting PbS QDs by employing crown ethers as a unique auxiliary additive.Experimental and theoretical investigations reveal that the formation of K^(+)-crown ethers complex effectively facilitates the dissociation of KCl in toluene and releases more Cl^(−)ions for extraordinary halide passivation at room temperature and in the air,thus improving the photoluminescence quantum yield from 24%to 35%in solution and further to 44%in blend films.The well-passivated PbS QD films are integrated with red organic light-emitting diodes(OLEDs)and the resulting QDOLEDs exhibit high-performance NIR emission centered at 887 nm,a high external quantum efficiency of 5.2%at a radiance of 10 W·sr^(−1)·m^(−2),superior operational stability with long lifetime T90 of 188 h at the current density of 25 mA·cm^(−2).We also construct a large-area NIR QD-OLED(5 cm×5 cm)with desirable uniform emission.This work opens a new avenue to achieve robust large-area NIR planar light sources for broad applications.
基金supported by the National Natural Science Foundation of China(21375132,21175138,21321003,21171114,91222202)the National Basic Research Program of China(2013CB834803)
文摘Protein protected gold nanoclusters have outstanding physical and chemical properties that make them excellent scaffolds for the construction of novel chemical and biological probes. In this study, a simple one-pot synthesis method was proposed for the preparation of fluorescent probes based on ovalbumin-stabilized gold nanoclusters. This strategy allowed the generation of water-soluble gold nanoclusters within 5 min. The as-prepared fluorescent probe exhibited a red fluorescence emission at 625 nm, and good thermostability. The fluorescent probe was applied to measure glucose concentrations based on the hydrogen peroxide-induced fluorescence quenching principle, and showed favorable biocompatibility, high sensitivity and good selectivity. As a result of the advantageous properties and performance of this fluorescent probe, the present assay allowed for the selective determination of glucose in the range of 5.0×10-6 to 10.0×10-3 mol/L with a detection limit of 1.0×10?6 mol/L. Moreover, the glucose content in urinary samples was analyzed using the constructed fluorescent probe: this indicated the potential of the fluorescent gold nanoclusters for applications in biological and clinical diagnosis and therapy.
基金financial support from the National Natural Science Foundation of China (Nos. 21575144, 91732103,21874138, 21727809, 21635008, 21621062)Chinese Academy of Sciences(No. QYZDJ-SSW-SLH034)
文摘Gold nanoclusters were rapid synthesized within 3 min at 120 ℃ by using papaya juice as a capping and reducing agent(P-AuNCs). The properties of the fluorescent probe were characterized by fluorescent spectroscopy, UV-vis spectroscopy, dynamic light scattering and transmission electron microscope.Based on the surface electron density increase-induced fluorescence enhancing principle, a high selective method for detection of L-lysine was developed with the as-prepared P-AuNCs coupling the fluorescence emission at 440 nm. The fluorescent probe showed high stability and good biocompatibility. Its fluorescence intensity was found to be linearly dependent on the L-lysine concentration in the range of 10.0μmol/L to 1000.0 μmol/L(R^2=0.969) with a limit of detection of 6.0μmol/L. Furthermore, the PAuNCs based approach was applied for monitoring the urine L-lysine contents, demonstrating great potential of fluorescent probes in real samples analysis.
基金the National Natural Science Foundation of China(Nos.22074148,21874138,21635008,21727809)。
文摘The temperature monitoring of treated cancer cells is critical in photothermal therapy.Current methods of detecting intracellular temperatures have low accuracy and poor spatial resolution,which limits their application to photothermal therapy.Herein,a strategy for targeted recognition and selective capture of MCF-7 breast cancer cells based on fluorescent polymer poly(N-isopropylacrylamide-benzoxadiazole-2-vinyl-4,4-dimethyl azlactone,PNMV)and modified gold nanobipyramids(Au NBPs-PNMV)was developed for temperature sensing during photothermal therapy.A mucin-1 protein aptamer(Apt)was applied to selectively target mucin-1 protein overexpressed on the surfaces of the MCF-7 cells,which can reduce interference by affinity interaction between the Apt and proteins.During photothermal therapy,the significant Au NBPs photothermal effect increases the fluorescence intensity of PNMV with temperature.Irradiation of MCF-7 cells cultured with Au NBPs-PNMV@Apt by an 808 nm laser increases the temperature of the system,while the cells can be inactivated because of the remarkable Au NBPs-PNMV@Apt photothermal effect.The results indicate that variation in the fluorescence of Au NBPs-PNMV@Apt can be applied as thermometers to monitor the intracellular effect of photothermal therapy.
基金the National Natural Science Foundation of China(51773109,21788102)National Key R&D Program of China(2020YFA0715001,2017YFA0204501)+1 种基金National Postdoctoral Program for Innovative Talents(BX20180159)the Project funded by China Postdoctoral Science Foundation(2019M660606)。
文摘Pursuing purely organic materials with high-efficiency near-infrared(NIR) emissions is fundamentally limited by the large nonradiative decay rates(k_(nr)) governed by the energy gap law. To date, reported endeavors to decelerate k_(nr) are mainly focused on reducing the electron-vibration coupling with the electronic nonadiabatic coupling assumed as a constant. Here, we demonstrated a feasible and innovative strategy by employing intermolecular charge-transfer(CT) aggregates(CTA) to realize high-efficiency NIR emissions via nonadiabatic coupling suppression. The formation of CTA engenders intermolecular CT in the excited states;thereby, not only reducing the electronic nonadiabatic coupling and contributing to small k_(nr) for high-efficiency NIR photoluminescence, but also stabilizing excited-state energies and achieving thermally activated delayed fluorescence for highefficiency NIR electroluminescence. This work provides new insights into aggregates and opens a new avenue for organic materials to overcome the energy gap law and achieve high-efficiency NIR emissions.
基金the financial support from the National Natural Science Foundation of China(Nos. 21575144, 21475137,21375132,21635008,21621062)Chinese Academy of Sciences(No. QYZDJ-SSW-SLH034)
文摘Ovalbumin-stabilized gold nanoclusters (OVA@AuNCs) were prepared with ascorbic acid as a reducing agent. This strategy could realize the synthesis of water-soluble OVA@AuNCs within 20 min. The asprepared fluorescent probe showed a red fluorescence emission at 630 nm. Moreover, the properties of the OVA@AuNCs were characterized by transmission electron microscope, dynamic light scattering, ultraviolet-visible spectroscopy, fluorescent spectroscopy. Based on the surface electron density decrease-induced fluorescence quenching mechanism, the OVA@AuNCs provided high sensitivity and selectivity for sensing copper ions. A good linear relationship was obtained between the fluorescence intensity of OVA@AuNCs and the concentration of copper ions in the range of 5.0-100.0pumol/L (R2z0.999) with a detection limit of 640 nmol/L. Furthermore, the rat serum copper contents were determined by using the OVA@AuNCs based assay, indicating great potential of fluorescent probes for application in biological and clinical analysis.
基金the financial support from the National Natural Science Foundation of China (Nos. 21575144, 91732103, 21874138, 21635008, 21621062)
文摘With _D-proline as the reducing and capping agent, fluorescent gold nanoclusters were rapidly prepared(_D-Pro@AuNCs) within 10 min at 100℃. In the present of gold nanoparticles, the fluorescence of _DPro@AuNCs was remarkably quenched. Interestingly, based on the electrostatic interaction between anticancer drug Raltitrexed and gold nanoparticles induced fluorescence "turn-on" principle, a high selective assay for detection of Raltitrexed was established with the probe associating the fluorescence emission at 435 nm. The fluorescence intensity of _D-Pro@AuNCs linearly correlated with the concentration of Raltitrexed in the range from 5.0 mmol/L to 40.0 mmol/L(R^2= 0.999) and the limit of detection was 1.9 mmol/L. Further, after Raltitrexed was abdominal injected in rats, a metabolic approach was constructed with the prepared fluorescent probe. It showed great potential of AuNCs-based sensing probes for application in analysis of serum anticancer drugs.
基金financial support from the National Natural Science Foundation of China (Nos. 21727809, 21635008, 21621062)Chinese Academy of Sciences(No. QYZDJ-SSW-SLH034)
文摘A new open-tubular capillary electrochromatography (OT-CEC) method for analysis of β-lactam antibiotics has been developed with unique block co-polymer coating. To obtain the highly ordered block polymer chains, reversible addition fragmentation chain transfer radical polymerization method was used to synthesize poly (maleic anhydride-styrene-N-isopropylacrylamide). The prepared block copolymer coating was characterized with NMR, fourier transform infrared spectroscopy and scanning electron microscope. Several key separation factors of OT-CEC, which including polymer amount,stability of the coating, temperature, species of organic additives, buffer pH and concentration, were investigated in detail. Our results indicated that the separation efficiency was improved greatly with the coating capillary and the three test analytes could be baseline separated. Then, the separation mechanism was briefly explored. Moreover, the proposed OT-CEC method displayed promising quantitative analysis property of the three test analytes with good linearity (R2>0.99), repeatability (relative standard deviations <0.9%) and high recovery (95.4%-106.2%). Further, the assay was applied in monitoring the three test β-lactam antibiotics (cephradine, cephalexin and amoxicillin) in serum samples, providing a useful platform for construction of novel polymer coatings in OT-CEC system and for analysis of drugs in real bio-samples.
基金the financial support from the National Natural Science Foundation of China(Nos.21874138,22074148,21727809,21635008)。
文摘Immobilization of enzymes onto carriers is a rapidly growing research area aimed at increasing the stability,reusability and enzymolysis efficiency of free enzymes.In this work,the role of phaseseparation and a pH-responsive"hairy"brush,which greatly affected the topography of porous polymer membrane enzyme reactors(PMER),was explored.The porous polymer membrane was fabricated by phase-separation of poly(styrene-co-maleic anhydride-acrylic acid)and poly(styrene-ethylene glycol).Notably,the topography and pores size of the PMER could be controlled by phase-separation and a pHresponsive"hairy"brush.For evaluating the enzymolysis efficiency of D-amino acid oxidase(DAAO)immobilized carrier(DAAO@PMER),a chiral ligand exchange capillary electrophoresis method was developed with D-methionine as the substrate.The DAAO@PMER showed good reusability and stability after five continuous runs.Notably,comparing with free DAAO in solution,the DAAO@PMER exhibited a17.7-folds increase in catalytic velocity,which was attributed to its tailorable topography and pHresponsive property.The poly(acrylic acid)moiety of poly(styrene-co-maleic anhydride-acrylic acid)as the pH-responsive"hairy"brush generated topography changing domains upon adjusting the buffer pH,which enable the enzymolysis efficiency of DAAO@PMER to be tuned based upon the well-defined architectures of the PMER.This approach demonstrated that the topographical changes formed by phaseseparation and the pH-responsive"hairy"brush indeed made the proposed porous polymer membrane as suitable supports for enzyme immobilization and fitting for enzymolysis applications,achieving high catalytic performance.
基金financially supported by the National Natural Science Foundation of China(21205125,21175138)
文摘Herein, a novel probe based on poly(N,N′-methylenebisacylamide) protected Au NPs(PDMAM-Au NPs) was developed for determination of silver ions. The thiol-terminated PDMAM was synthesized by the reversible addition fragmentation chain transfer radical polymerization. Then, the PDMAM-Au NPs were prepared by a simple, one-pot and green process. It has been observed that existence of the silver ions evoked a small red-shift to the emission peak of PDMAM-Au NPs and an obvious increase in UV absorption. The detection limit of the present method for silver ions was 0.5 ?mol/L, with a linear range of 1.0–1000 ?mol/L. Moreover, the possible mechanism for enhanced UV absorption intensity with enlarged diameter of PDMAM-Au NPs was explored and discussed briefly. The results demonstrated that silver ions could be detected by the PDMAM-Au NPs based colorimetric assays, further opening up new ways for the visualization and quantification of silver ions involved in our daily life.
基金supported by the National Key R&D Program of China(grant nos.2016YFB0401003 and 2016YFB0400702)the National Science Fund of China(grant no.51525304).
文摘The operational stability of organic(opto)electronic devices largely depends on the intrinsic stability of organic materials on service.For organic light-emitting diode(OLED)materials,a key parameter of their intrinsic stability is the bond-dissociation energy of the most fragile bond(BDE_(f)).Although rarely involved,many OLED molecules have the lowest BDE_(f) in anionic states[BDE_(f)(−)∼1.6–2.5 eV],which could be a fatal short-slab for device stability.Herein,we separated BDE_(f)(−)from other parameters and confirmed the clear relationship between BDE_(f)(−),intrinsic material stability and device lifetime.Based on thermodynamic principles,we developed a general and effective strategy to greatly improve BDE_(f)(−)by introducing a negative charge manager within the molecule.The manager must combine an electron-withdrawing group(EWG)with a delocalizing structure,so that it can firmly confine the negative charge and hinder the charge redistribution toward fragile bonds.Consequently,the use of this manager can substantially promote BDE_(f)(−)by∼1 eV for various fragile bonds and outperform the effect reported from solely employing EWGs or delocalizing structures.This effect was verified in typical phosphine-oxide and carbazole derivatives and backed up by newly designed molecules with multiple fragile bonds.This strategy provides a new way to transform vulnerable building blocks into robust organic(opto)electronic materials and devices.