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Study Of Novel Bioanalysis Methods Based On Perovskite Nanocrystals

Posted on:2022-10-01Degree:DoctorType:Dissertation
Country:ChinaCandidate:M L LiFull Text:PDF
GTID:1480306725471604Subject:Biology
Abstract/Summary:PDF Full Text Request
In order to discover the laws of human life activities,make early diagnosis of human diseases, and obtain more comprehensive biological information,proteins,peptides,bioactive small molecules and toxic environmental pollutants that are closely related to life activities.Recently,innovations in nanomaterials have continued to emerge,providing strong support and unprecedented development changes for the development and establishment of new methods of bioanalysis.As a result,the research on new methods of bioanalysis based on nanomaterials is one of the most active research in bioanalysis.The development of new nanomaterials is well-established,efficient,high-performance,small,and easy-to-use miniaturization Biochemical analysis methods have opened the situation,which has greatly contributed to the development of precision medicine,medicine and health,environmental testing,forensic identification and other related research fields.Perovskite nanocrystals have excellent physical and chemical properties,including ultra-high fluorescence quantum yield,adjustable emission wavelength,easy synthesis,and have received great concern and attention international attention.In consideration of their unique advantages and huge success in optoelectronics,one may envision perovskite nanocrystals would also hold great potential for biological applications.Therefore,this paper focuses on the the development of a series of novel bioanalytical strategies,these are based on perovskite nanomaterial as scaffold and biomolecule as functional elements for detecting proteins,peptides,biologically small molecules and biotoxin.Through the analysis of real samples,we have preliminarily demonstrated that the feasibility and dominance of perovskite nanomaterial in bioanalysis compared with traditional test methods.The detailed content is described as follows:1.One-step assay of pore-forming biotoxins based on perovskite nanocrystalsAs one of the emerging inorganic materials,perovskite nanocrystals(NCs)have inspired the development of various optoelectronic applications in recent years;however the effective utilization in biomedical fields is still limited.Herein,we report a quantitative measurement of broad-spectrum pore-forming toxins in complex media based on biomimetic CsPbBr3 NCs.Specifically,by coating CsPbBr3 NCs with phospholipid(PM-CsPbBr3 NCs),the outer micelle membrane can not only serve as a shell to protect the stability of CsPbBr3 NCs,but also interact with broad-spectrum biotoxins.Meanwhile,toxin-triggered transmembrane pore formation can cause water permeation,which breaks down the structure of PM-CsPbBr3 NCs,generating striking fluorescent and electrochemical dual responses.Therefore,direct quantitative measurements of biotoxins are realized via dual-readout signals with inverse change trend,resulting in a detection limit of 50 nM.Our report represents the first example of CsPbBr3 NCs for the develpment of building biosensors.Meanwhile,such a label-free,cost-effective and widely applicable biomimetic PM-CsPbBr3 NCs may present a valuable tool for the detection of biotoxin infections,and overcome the limitations of perovskite materials in biosensing.2.Dynamic monitoring and analysis method of H2O2 based on perovskite nanocrystalsAll-inorganic lead halide perovskite nanocrystals(CsPbBr3 NCs)have excellent optical properties and drawn considerable attention in recent years.Herein,for the first time,we discover that phospholipid membrane(PM)-encapsulated CsPbBr3 NCs(PM-CsPbBr3 NCs)have biocatalytic activity,we realized that CsPbBr3 NCs,as a new type of nanozyme,their own fluorescence signal changes are also attractive.When H2O2 is present,the fluorescence signal of PM-CsPbBr3 NCs is quickly quenched.When the H2O2 is removed,the fluorescence signal is restored.The whole process does not require the additional chromogenic reagents(e.g TMB),which can reflect the process of H2O2 catalytic reaction based on“add-to-answer”biosensing mode.So,we have designed PM-CsPbBr3 NCs as a new type of nanoreporter for real-time monitoring of H2O2 metabolism in an enclosed biological environment(such as,in He La cells and zebrafish),which greatly broadened the application of CsPbBr3 NCs in biological analysis.We envision that CsPbBr3 NCs,as a self-feedback nanozyme without external chromogenic reagents,deepen people's understanding of nanozymes,and drive their new understanding in the fields of disease diagnosis,biosensing and bioimaging.3.Visual analysis method of several metabolites based on perovskite nanocrystalsAll-inorganic CsPbX3 perovskite nanocrystals,with excellent optical properties,have drawn considerable attention in recent years.However,because of their poor aqueous stability,non-targeting ability and potential toxicity,it remains a big challenge to apply perovskite nanocrystals in complex matrixes.We discover that the phospholipid membrane(PM)-coated CsPbX3 NCs have intrinsic biocatalytic activity,which can report H2O2 concentration in biofluids.After thoroughly investigating the lipid composition and combination,PM-CsPbX3 NCs with enhanced aqueous stability and biocompatibility can be obtained,which can be used as a robust peroxidase-like nanozyme.Notably,the fluorescence of PM-CsPbX3 NCs can be rapidly quenched by adding H2O2 and then restored by removing excess H2O2.Initiated from this unexpected observation,we have tried to assemble the oxidases on the outer layer of the nanomaterial PM-CsPbX3 NCs,namely oxidases/PM-CsPbX3 NCs,to realize the functionalization of PM-CsPbX3 NCs.Next,PM-CsPbX3 NCs can be explored as a tandem enzyme system for the detection of kinds of important metabolites in human biofluids(including blood,urine and sweat).In order to detect biomarkers under different testing occasions with good field-deployment capability,oxidases/PM-CsPbX3 NCs are prepared into fluorescent paper-based analysis test,which can be stored for a long period.They are convenient-to-implemented,and the test results can be directly distinguished by naked eyes.This work is not only the first report on the discovery of nanozyme-like property of all-inorganic perovskite CsPbX3NCs,but also demonstrates the great potential of CsPbX3 NCs in bioanalysis,which drive new understanding in biocatalysis and open avenues for diagnostics and biosensing.4.An individual Cloud-based platform for latent fingerprint identification based on perovskite nanocrystalsFingerprint formed through lifted papillary ridges is considered as the best reference for personal identification.However,the currently available latent fingerprint(LFP)images often suffer poor-resolution,low-degree information,and require multifarious steps for identification.Herein,an individual Cloud-based fingerprint operation platform has been designed and fabricated to achieve high-definition latent figerprints analysis by using CsPbX3 perovskite nanocrystals(NCs)as eikonogen.Moreover,since CsPbX3 NCs have a special response to some fingerprint-associated amino acids,the proposed platform can be further used to detect metabolites on latent figerprints.Consequently,in virtue of Cloud computing and artificial intelligence(AI),this study has demonstrated a champion platform to realize the whole latent figerprints identification analysis.In a double-blind simulative crime game,the enhanced LFP images can be easily obtained and used to lock the suspect accurately within one second on a smartphone,which can help investigators track the criminal clue and handle cases efficiently.
Keywords/Search Tags:Perovskite nanocrystals, biochemical analysis, biotoxins, electrochemical detection, fluorescent detection, hydrogen peroxide, nanoreporter, visual analysis, fingerprint identification
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