Naslov (srp)

Elektrogenerisana hemiluminiscencija: ispitivanje mehanizma i njena primena u bioanalitici : doktorska disertacija

Autor

Sentić, Milica N., 1987-

Doprinosi

Manojlović, Dragan. 1961-
Šojić, Nešo
Roglić, Goran, 1964-

Opis (eng)

Electrogenerated chemiluminiscence (ECL) is a process which emits luminiscent signals by converting electrochemical energy into radiative energy. It offers very sensitive detection of sub-picomolar concentrations with an extremely large dynamic range, greater than six orders of magnitude and almost zero background signal. The direct optical readout can be performed just with a photomultiplier tube (PMT) or inexpensive CCD cameras and therefore, easily combined with other technologies such as microfluidics and capillary electrophoresis to obtain complete detection systems. ECL detection is widely used in commercialized systems with an increasing trend. The present thesis is aimed at studying the fundamental ECL process and at developing new ECL systems for original bioanalytical applications. Chapter one is dedicated to the general principles of ECL. Two different pathways to generate ECL, annihilation and co-reactant ECL, are explained in details. The most used ECL luminophores, based on ruthenium complexes, and co-reactants are also presented. In the last part 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 and their influence on ECL emission were investigated. Spectroelectrochemistry and ECL imaging was combined to observe the ECL generation from a single micro-bead, functionalized with ruthenium 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 such a 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 electrochemical characteristic that makes the NEEs very useful in the development of chemical nanosensors is the dramatic lowering of capacitive currents (that are the largest component of the noise, or more properly the background signal of voltammetric measurements) allowing very sensitive detection of analytes of interest. Exploiting both gold NEEs as a sensor platform and generation of ECL at low oxidation potentials, a new sensitive and specific ECL immunosensor for diagnosis of celiac disease (CD) will be presented. In the last chapter, principles of bipolar electrochemistry (BE) will be presented. This concept has been recently used to control the motion of autonomous microswimmers, breaking the symmetry on the surface of this conductive objects in a wireless manner. The strategy to trigger the motion relies on the generation and release of bubbles and was used for translation, rotation and levitation and it will be described in details. We will present the integration of ECL light...

Opis (srp)

U okviru ove doktorske disertacije ispitana je elektrogenerisana hemiluminiscencija (eng. Electrogenerated chemiluminiscence - ECL) kao i razvoj novih ECL sistema za bioanalitičku primenu. ECL je metoda u kojoj se analitički signal u vidu luminiscentnog zračenja, dobija putem elektrohemijske reakcije indukovane na površini elektorde. ECL omogućava veoma preciznu detekciju u subpikomolarnim opsegu koncentracija sa gotovo nultim pozadinskim signalom. Direktno optičko očitavanje može se izvršiti veoma jednostavno pomoću fotomultiplikatorskih cevi (eng. photomultiplier tube - PMT) ili jeftinih CCD (eng. charge coupled device - CCD) kamera. Zbog toga se ECL može lako kombinovati sa drugim tehnologijama kao što su mikrofluidni sistemi i kapilarna elektroforeza u cilju dobijanja kompletnog sistema za detekciju. ECL detekcija se široko koristi u komercijalizovanim sistemima. Ova teza ima za cilj proučavanje osnovnih ECL procesa kao i razvoj inovativnih ECL sistema za bioanalitičku primenu. Prvo poglavlje je posvećeno opštim principima ECL–a. Dva različita mehanizma za generisanje ECL-a (anihilacija i ECL pomoću koreaktanata (eng. co-reactant)) su objašnjeni do detalja. Najčešće korišćene ECL luminofore, bazirane na kompleksima rutenijuma, kao i sve vrste korektanata, su takođe opisane. Na kraju, glavne primene elektrohemijske luminiscencije su ukratko prikazane. U drugom poglavlju, proučavani su ECL mehanizmi zastupljeni u imunotestovima u kojima su platforme za ECL detekciju bazirane na česticama mikrometarskih dimenzija. Ispitan je učinak različitih ECL mehanizama na ukupan intenzitet emitovanog ECL signala. Spektroelektrohemija i ECL snimanje su kombinovani za posmatranje generisanja ECL na nivou jedne mikrosfere, funkcionalizovane kompleksom rutenijuma sa dva koreaktanta, pomoću prostornog mapiranja ECL reaktivnosti. Ovaj novi pristup snimanja ECL signala pruža uvid u ECL mehanističke rute koji omogućavaju izuzetno visoku osetljivost komercializovanim biotestovima baziranim na korisćenju mikrosfera/mikroperli. Treće poglavlje govori o elektrohemijskim osobinama nanoelektroda (eng. nanoelectrode ensembles - NEEs), i najnovijem napretku na polju njihove pirmene u bioelektroanalitičkoj hemiji. Elektrohemijske osobine koje čine NEEs veoma korisnim u razvoju hemijskih...

Opis (srp)

Hemija / Chemistry Datum odbrane: 04.05.2016.

Jezik

srpski

Datum

2016

Licenca

Creative Commons licenca
Ovo delo je licencirano pod uslovima licence
Creative Commons CC BY-NC-ND 2.0 AT - Creative Commons Autorstvo - Nekomercijalno - Bez prerada 2.0 Austria License.

http://creativecommons.org/licenses/by-nc-nd/2.0/at/legalcode

Predmet

OSNO - Opšta sistematizacija naučnih oblasti, Instrumentalne metode

electrogenerated chemiluminiscence, 3D ECL imaging, immunoassays,nanoelectrode ensenbles, bipolar electrochemistry, analytical swimmers

OSNO - Opšta sistematizacija naučnih oblasti, Instrumentalne metode

elektrogenerisana hemiluminiscencija, 3D ECL prikaz, imunotestovi, skupunenano-elektroda, bipolarna elektrohemija, analitički plivači