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Electrogenerated chemiluminescence: from mechanistic insights to bioanalytical applications

dc.contributor.advisorManojlović, Dragan
dc.contributor.otherŠojić, Nešo
dc.contributor.otherRoglić, Goran
dc.creatorSentić, Milica
dc.date.accessioned2019-02-04T12:27:30Z
dc.date.available2019-02-04T12:27:30Z
dc.date.issued2016
dc.identifier.urihttp://eteze.bg.ac.rs/application/showtheses?thesesId=3446
dc.identifier.urihttps://fedorabg.bg.ac.rs/fedora/get/o:12027/bdef:Content/download
dc.identifier.urihttp://vbs.rs/scripts/cobiss?command=DISPLAY&base=70036&RID=48107535
dc.identifier.urihttp://nardus.mpn.gov.rs/123456789/6117
dc.identifier.urihttps://cer.ihtm.bg.ac.rs/handle/123456789/2577
dc.description.abstractU okviru ove doktorske disertacije ispitana je elektrogenerisana hemiluminiscencija (eng.Electrogenerated chemiluminiscence - ECL) kao i razvoj novih ECL sistema za bioanalitičkuprimenu. ECL je metoda u kojoj se analitički signal u vidu luminiscentnog zračenja, dobijaputem elektrohemijske reakcije indukovane na površini elektorde. ECL omogućava veomapreciznu detekciju u subpikomolarnim opsegu koncentracija sa gotovo nultim pozadinskimsignalom. Direktno optičko očitavanje može se izvršiti veoma jednostavno pomoćufotomultiplikatorskih cevi (eng. photomultiplier tube - PMT) ili jeftinih CCD (eng. chargecoupled device - CCD) kamera. Zbog toga se ECL može lako kombinovati sa drugimtehnologijama kao što su mikrofluidni sistemi i kapilarna elektroforeza u cilju dobijanjakompletnog sistema za detekciju. ECL detekcija se široko koristi u komercijalizovanimsistemima. Ova teza ima za cilj proučavanje osnovnih ECL procesa kao i razvoj inovativnihECL sistema za bioanalitičku primenu.Prvo poglavlje je posvećeno opštim principima ECL–a. Dva različita mehanizma za generisanjeECL-a (anihilacija i ECL pomoću koreaktanata (eng. co-reactant)) su objašnjeni do detalja.Najčešće korišćene ECL luminofore, bazirane na kompleksima rutenijuma, kao i sve vrstekorektanata, su takođe opisane. Na kraju, glavne primene elektrohemijske luminiscencije suukratko prikazane.U drugom poglavlju, proučavani su ECL mehanizmi zastupljeni u imunotestovima u kojima suplatforme za ECL detekciju bazirane na česticama mikrometarskih dimenzija. Ispitan je učinakrazličitih ECL mehanizama na ukupan intenzitet emitovanog ECL signala.Spektroelektrohemija i ECL snimanje su kombinovani za posmatranje generisanja ECL nanivou jedne mikrosfere, funkcionalizovane kompleksom rutenijuma sa dva koreaktanta,pomoću prostornog mapiranja ECL reaktivnosti. Ovaj novi pristup snimanja ECL signala pružauvid u ECL mehanističke rute koji omogućavaju izuzetno visoku osetljivost komercializovanimbiotestovima baziranim na korisćenju mikrosfera/mikroperli.Treće poglavlje govori o elektrohemijskim osobinama nanoelektroda (eng. nanoelectrodeensembles - NEEs), i najnovijem napretku na polju njihove pirmene u bioelektroanalitičkojhemiji. Elektrohemijske osobine koje čine NEEs veoma korisnim u razvoju hemijskih...sr
dc.description.abstractElectrogenerated chemiluminiscence (ECL) is a process which emits luminiscent signals byconverting electrochemical energy into radiative energy. It offers very sensitive detection ofsub-picomolar concentrations with an extremely large dynamic range, greater than six ordersof magnitude and almost zero background signal. The direct optical readout can be performedjust with a photomultiplier tube (PMT) or inexpensive CCD cameras and therefore, easilycombined with other technologies such as microfluidics and capillary electrophoresis to obtaincomplete detection systems. ECL detection is widely used in commercialized systems with anincreasing trend. The present thesis is aimed at studying the fundamental ECL process and atdeveloping new ECL systems for original bioanalytical applications.Chapter one is dedicated to the general principles of ECL. Two different pathways to generateECL, annihilation and co-reactant ECL, are explained in details. The most used ECLluminophores, based on ruthenium complexes, and co-reactants are also presented. In the lastpart of this chapter, the principal applications of ECL are briefly described.In the second chapter, the study of ECL mechanisms used in bead-based immunoassays andtheir influence on ECL emission were investigated. Spectroelectrochemistry and ECL imagingwas combined to observe the ECL generation from a single micro-bead, functionalized withruthenium complex with two efficient co-reactants, by mapping the ECL reactivity in space.This new imaging approach provides insights into the ECL mechanistic route operating in sucha commercialized bead-based bioassays and its extremely high sensitivity.Chapter 3 addresses the electrochemical properties of nanoelectrode ensembles and arrays(NEEs) with recent advances in bioelectroanalytical applications. The electrochemicalcharacteristic that makes the NEEs very useful in the development of chemical nanosensors isthe dramatic lowering of capacitive currents (that are the largest component of the noise, ormore properly the background signal of voltammetric measurements) allowing very sensitivedetection of analytes of interest. Exploiting both gold NEEs as a sensor platform and generationof ECL at low oxidation potentials, a new sensitive and specific ECL immunosensor fordiagnosis of celiac disease (CD) will be presented.In the last chapter, principles of bipolar electrochemistry (BE) will be presented. This concepthas been recently used to control the motion of autonomous microswimmers, breaking thesymmetry on the surface of this conductive objects in a wireless manner. The strategy to triggerthe motion relies on the generation and release of bubbles and was used for translation, rotationand levitation and it will be described in details. We will present the integration of ECL light...en
dc.formatapplication/pdf
dc.languagesr
dc.publisherУниверзитет у Београду, Хемијски факултетsr
dc.rightsopenAccess
dc.rights.urihttps://creativecommons.org/licenses/by-nc-nd/4.0/
dc.sourceУниверзитет у Београдуsr
dc.subjectelektrogenerisana hemiluminiscencijasr
dc.subjectelectrogenerated chemiluminiscenceen
dc.subject3D ECL prikazsr
dc.subjectimunotestovisr
dc.subjectskupunenano-elektrodasr
dc.subjectbipolarna elektrohemijasr
dc.subjectanalitički plivačisr
dc.subject3D ECL imagingen
dc.subjectimmunoassaysen
dc.subjectnanoelectrode ensenblesen
dc.subjectbipolar electrochemistryen
dc.subjectanalytical swimmersen
dc.titleElektrogenerisana hemiluminiscencija: ispitivanje mehanizma i njena primena u bioanaliticisr
dc.titleElectrogenerated chemiluminescence: from mechanistic insights to bioanalytical applicationsen
dc.typedoctoralThesisen
dc.rights.licenseBY-NC-ND
dcterms.abstractМанојловић, Драган; Шојић, Нешо; Роглић, Горан; Сентић, Милица Н.; Електрогенерисана хемилуминисценција: испитивање механизма и њена примена у биоаналитици; Електрогенерисана хемилуминисценција: испитивање механизма и њена примена у биоаналитици;
dc.identifier.rcubhttps://hdl.handle.net/21.15107/rcub_nardus_6117
dc.identifier.fulltexthttps://cer.ihtm.bg.ac.rs/bitstream/id/8892/2575.pdf
dc.type.versionpublishedVersion


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