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Development And Application Of Electrochemiluminescence Biosensors Based On Organic Composite Materials

Posted on:2022-03-09Degree:MasterType:Thesis
Country:ChinaCandidate:Y LuFull Text:PDF
GTID:2511306476994929Subject:Physical chemistry
Abstract/Summary:PDF Full Text Request
Electrochemiluminescence(ECL)mainly refers to the phenomenon that the luminescent substance on the electrode surface can produce light signal through redox reaction.In recent years,the research of electrochemiluminescence sensor is more and more in-depth,which is mainly based on the advantages of low background signal,wide linear range and low detection limit of electrochemiluminescence sensor.It is constantly explored and innovated,especially in clinical analysis,pesticide detection,DNA analysis,immune analysis and other fields.Aggregation induced electrochemiluminescence is a kind of luminescent phenomenon which has been studied more and more in recent years.The phenomenon that the energy consumed by the vibration and rotation of molecules can be minimized by using the organic matter in the aggregation state,so as to enhance the fluorescence and further enhance the electrochemiluminescence.In this paper,pt-tio2-ptc and g-c3n4-au-luminol were used to construct a sandwich quenched electrochemiluminescence sensor,and triphenylaldehyde was designed and synthesized to explore the aggregation induced fluorescence and enhanced electrochemiluminescence of triphenylaldehyde in different environments.The main research contents are as follows:(1)A quenching sensor using perylene tetracarboxylic anhydride derivative complex(PT-Ti O2-PTC)as the ECL luminophore was successfully constructed,in which C60-BSA was used as the matrix and glucose oxidase(GOx)was used as the specific recognition site.In order to reduce the high photoelectron-hole recombination rate of Ti O2,a Pt-Ti O2 composite material was synthesized to improve the catalytic performance of Ti O2,and to further enhance the ECL signal of sensing.C60 has electrophilic reaction activity,so it easily reacts with electron-rich substances.Therefore,the BSA-C60 composite material was prepared as the matrix,the surface of which was rich in carboxyl and amino groups,and the formation of amide bonds to promote further combination with other substances.The larger specific surface area of BSA-C60 can combine with more luminescent materials to enhance ECL intensity.At the same time,C60can also interact with K2S2O8 to generate more SO4.-radicals,further enhancing the electrochemiluminescence signal.When different concentrations of concanavalin(Con A)are connected to the electrode through an immune reaction,the detected electrochemiluminescence intensity changes,so as to realize the sensitive detection of Con A.Under the optimal conditions,the constructed biosensor exhibited excellent Con A detection performance with the lowest detection limit of 1.81×10-5 ng/m L.The prepared sensor has the advantages of wider linear range,lower detection limit,good selectivity,which provides a new method for the detection of Con A.(2)A double-enhancement quenching aptamer electrochemiluminescence sensor was successfully constructed to realize the sensitive detection of human mucin 1(mucin1).The synthesized g-C3N4-Au-luminol is used as an electrochemiluminescence probe,which is not easy to fall off on the electrode surface and the luminescence signal is stable.At the same time,the synthesized Zn Cu S semiconductor material has a strong catalytic effect on hydrogen peroxide,can catalyze the production of a large amount of.OH and O2.-,then react with luminol in the system to produce a large amount of luminol*.In the process of luminol*returning from the excited state to the ground state,generate electrochemiluminescence signal.Through the specific recognition of the aptamer,mucin1 in the system can easily capture,causing the electrochemiluminescence signal changes significantly.Under the optimal conditions,the sensor showed significant mucin1 detection performance at 10-4-103 ng/m L,and the LOD was 5.04×10-5 ng/m L.(3)The electrochemiluminescence of triphenylamine aldehyde-malononitrile complex is studied based on the principle of aggregation-induced luminescence.The aggregation-induced luminescence is mainly by inhibiting the internal vibration and rotation of the molecule to inhibit energy loss.In this experiment,the triphenylamine aldehyde-malononitrile complex was successfully synthesized to study its fluorescence enhancement effect in the water/dimethyl sulfoxide(H2O/DMSO)system and the bovine serum albumin(BSA)system.The solubility of triphenylamine aldehyde-malononitrile in aqueous solution is very poor.When it is dissolved with different proportions of H2O/DMSO,the aggregation effect in the system is different.With the increase of water content,the fluorescence effect becomes stronger and stronger.The intensity of electrochemiluminescence is also gradually increasing,in line with the expectations of the experiment.At the same time,BSA itself has hydrophobic and hydrophilic groups.When BSA is mixed with organics,the hydrophobic part wraps the complex together and restricts the vibration and rotation of the groups in the molecule.The experiment successfully confirmed that the aggregation induction can also be observed through the BSA system.Therefore,combining the aggregation induction effect with electrochemiluminescence in this experiment provides a new idea for the study of electrochemiluminescence probes.
Keywords/Search Tags:electrochemiluminescence aptamer sensor, luminol, mucin 1, aggregation induced luminescence, concanavalin A
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