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Electrogenerated Chemiluminescence of Gold Nanoclusters
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Electrogenerated Chemiluminescence of Gold Nanoclusters
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Dissertation
Electrogenerated Chemiluminescence of Gold Nanoclusters
2014
Overview
A series of monodispersed AuNCs (size < 2 nm) including Au144(SR)60, Au38(SR)24 and Au25(SR)18z (z =1-, 0 and 1+, SR=2-phenylethanethiol) were prepared. All these nanoclusters showed molecule-like optical and electrochemical properties. These two features are essential for an electrogenerated chemiluminescence or electrochemiluminescence (ECL) study. The Au144(SR)60 showed a small HOMO-LUMO gap determined by electrochemistry. No ECL light was seen in the annihilation process, while NIR ECL was observed with tri-n-propylamine (TPrA) (Chapter 2). ECL was highly efficient in the Au38(SR)24/TPrA co-reactant system. This nanocluster also showed ECL emission with benzoyl peroxide (BPO), while no ECL was detected in the annihilation route (Chapter 3). The ECL of Au25(SR)18z (z =1-, 0 and 1+) were discovered to emit NIR ECL light in the presence of either TPrA or BPO co-reactant. The Au25(SR)18+ / TPrA system revealed the strongest ECL emission among the three Au25 oxidation states (Chapter 4). The thermodynamic (Latimer-type diagram) and the kinetic origins of Au25(SR)18 0 ECL were explored in the presence of TPrA (Chapter 5). And lastly, the NIR ECL of Au25(SR)18− nanoclusters was mechanistically investigated in the presence of both TPrA and BPO with NIR emissions in both systems (Chapter 6).In each case multiple ECL emissions were observed. The ECL peak wavelength and ECL intensity can be tuned by means of both the co-reactant concentration and applied electrode potential. It is worth noting that the Au38(SR)24 showed the strongest ECL efficiency among all the clusters studied, and the Au25(SR)18z clusters possessed a rich photoelectrochemistry leading to highly efficient ECL.
