Research And Application Of Luminescence Analysis Based On Cu-MOFs/Fe-MOFs On Paper Chips

Metal-organic frameworks?MOFs?,as a new class of hybrid materials with high porous structure,are synthesized by metal ion or clusters and organic ligands.With the advantages of large surface area and structural flexibility,MOFs have gain unparalleled attention for the construction of biosensors.However,the chemilumescence property with MOFs on the paper and MOFs using as the detection antibody label are seldom reported.In this thesis,the chemiluninescent property with copper-MOFs was investigated on the paper-based chip and a "glow" type of Iuminol CL system was developed.Also,the paper-based immunodevice with MOFs using as the antibody label was constructed by the CL and fluorescence double detection mode.This thesis is divided into two parts,the first part is the review,which composed of the concept of MOFs and its application in luminescenceThe second part is as follows:1.Investigation on paper-based chip with Cu-MOFs catalyzed luminol-H₂O₂ chemiluminescence systemCu-PDA metal-organic frameworks,which composed of Cu???and 1,10-phenanthroline-2,9-dicarboxylic acid?PDA?was synthesized by a simple method at room temperature in this work.Thecatalytic performance with Cu-PDA in luminol-H₂O₂ CLsystem was investigated on paper.The results showed that Cu-PDA had a high catalytic activity for this CL system.The chemiluminescence signal produced slowly on paper and the maximum chemiluminescence intensity can be produced at 4 mins,then the CLintensity declined gradually.The whole procedure for luminescencecan last for over 10 mins.The chemiluminescence imaging signals on paper were also recorded..The possible CL mechanism was discussed according to electron paramagnetic resonance?EPR?and the experiments with the effects of radical scavengers on Cu-MOF catalyzed luminol-H₂O₂ CL system.The results suggested that the CL emission of this system might derive from the oxidation reaction of luminol by reactive oxygen species?including singlet oxygen,hydroxyl radicals and superoxide anion radicals?,which produced in the process of the decomposition of H₂O₂ catalyzed by Cu-MOFs.This work open up the promising application of MOFs in chemiluminescence,and provide guidance for the future application in this field.2.Investigation of a chemiluminescence and fluorescence dual detection mode paper-based immunosensor with Fe-MOFs as the antibody labelIn this wok,a metal-organic frameworks with Fe-MOFs,consisting of Fe3+ and 2-aminobenzene-1,4-dicarboxylic acid?NH2-BDC?,was rapidly and mildly synthesized at room temperature.The Fe-MOFs showed a strong fluorescent signal and catalytic capacity for luminol-H₂O₂ chemiluminescence system.Fe-MOFs showed an emission wavelength of 430 nm under excitation of a 300 nm source.The active group-NH2 on the surface of Fe-MOFs was beneficial for the connection of Fe-MOFs with the prostate specific antigen?PSA?detection antibody through the linker of glutaraldehyde.The Fe-MOFs was used as a signal antibody label for the detection of PSA on paper-based immune-devices,and a paper-based chemiluminescence and fluorescence dual mode immunosensor was developed for the detection of PSA.The PSA detection limits of chemiluminescence and fluorescence method were 0.3 ng mL^-1 and 0.2 ng mL^-1 The linear ranges were 0.5-30 ng mL^-1 and 1-30 ng mL^-1,respectively.In this work,a paper-based immune-device with fluorescence and chemiluminescence double detection mode was established by using MOFs materials.This strategy enriches and expands the development and application of MOFs materials in field of paper-based devices.3.Inkjet printing paper-based immunodevice for fluorescence determination of Immunoglobulin GA sequential inkjet printing strategy was utilized on a micro fluidic paper-based fluorescence?FL?immunodevice for Immunoglobulin G?IgG?detection.Assisted with four cartridges,capture antibody,antigen and detection antibody were sequentially printed on the paper surface to complete the IgG detection.For enzyme-linked immunosorbent assay?ELISA?,the analysis time and reagent consumption were significantly decreased in comparison to traditional manually pipetting.IgG can be detected with a better reproducibility and the detection limit was 0.4 ng mL^-1.Besides,size effect of gold nanoparticles?AuNPs?was also investigated by the inkjet printer's nozzle,and the particle diameter of less than 150 nm can be successfully printed on the paper surface without affecting the detection results.This work will provide a new strategy of little volume reagents consumption and large-scale sample detection in the field of immunoassay.