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Sinteza in uporaba plazmonskih katalizatorjev na osnovi Au+TiO(sub)2 za fotokatalitsko oksidacijo organskih onesnažil ob uporabi vidne svetlobe
ID Dolhar, David (Author), ID Sollner Dolenc, Marija (Mentor) More about this mentor... This link opens in a new window, ID Žerjav, Gregor (Co-mentor)

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Abstract
Onesnaženje čistih voda že od začetka pospešene industrializacije predstavlja enega od glavnih problemov človeštva. Organizacija združenih narodov ocenjuje, da je na svetu več kot miljarda ljudi brez dostopa do čiste vode, ki bi bila varna in primerna za pitje. Poseben problem predstavljajo persistentna onesnaževala, ki se v velikih količinah uporabljajo v mnogih industrijskih panogah. Med taka onesnaževala sodijo tudi motilci endokrinega sistema, natančneje bisfenoli, ki lahko že v majhnih količinah vplivajo na fiziološke procese v človeškem organizmu. V zadnjih letih so se napredni oksidacijski procesi izkazali kot učinkovito orodje za odstranjevanje persistentih onesnaževal iz odpadnih voda. Širok nabor naprednih oksidacijskih procesov omogoča prilagajanje postopkov oksidacije zahtevanim specifikacijam za razgradnjo onesnaževal. Za čiščenje voda je še posebej primerna heterogena fotokataliza z uporabo fotokatalitsko aktivnega TiO2. V okviru raziskovalnega dela magistrske naloge smo pripravili plazmonske katalizatorje na osnovi Au+TiO2, pri čemer smo kot izhodiščni material uporabili TiO2 nanodelce in nanopalčke, ki smo jih proizvedli po postopku alkalne hidrotermalne sinteze. Zlato smo na delce TiO2 nanesli z metodo depozicije in precipitacije. Ovrednotili smo fizikalno-kemijske lastnosti Au+TiO2 materialov in njihovo fotokatalitsko aktivnost pod vidno svetlobo. Pripravljene katalizatorje smo uporabili v procesih fotokatalitske oksidacije štirih različnih tipov bisfenolov (bisfenola A, S, AF in F) pod vidno svetlobo. Koncentracijo onesnaževal med reakcijami smo spremljali s tekočinsko kromatografijo visoke ločljivosti, stopnjo mineralizacije onesnaževal pa smo določili z merjenjem količine celotnega organskega ogljika pred in po reakcijh fotokatalitske razgradnje. Ugotovili smo, da se Au+TiO2 nanopalčke in Au+TiO2 nanodelci med seboj razlikujejo v fizikalno-kemijskih lastnostih in po fotokatalitski aktivnosti pod vidno svetlobo. Prisotnost zlata na površini katalizatorja pomembno vpliva na njegovo fotokatalitsko aktivnost pod vidno svetlobo. Ugotovili smo tudi, da imajo Au+TiO2 katalizatorji ugodne lastnosti za razgradnjo bisfenolov kot modelnih organskih onesnaževal. Au+TiO2 nanopalčke so se v primerjavi z Au+TiO2 nanodelci izkazale kot bolj učinkovit katalizator. Pri oksidaciji BPF je bil ob uporabi Au+TiO2 nanopalčk odstotek razgradnje v dveh urah približno 95 %, pri BPA približno 80 %, pri BPS nekaj več kot 20 %, pri BPAF pa nekaj manj kot 20 %. Razgradnja BPS in BPAF je še posebej zahtevna zaradi njunih specifičnih strukturnih elementov.

Language:Slovenian
Keywords:Heterogena fotokataliza, Au+TiO2 fotokatalizatorji, napredni oksidacijski procesi, motilci endokrinega sistema, bisfenoli.
Work type:Master's thesis/paper
Organization:FFA - Faculty of Pharmacy
Year:2020
PID:20.500.12556/RUL-119371 This link opens in a new window
Publication date in RUL:08.09.2020
Views:1439
Downloads:191
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Secondary language

Language:English
Title:Surface plasmon resonance enabled activity of Au+TiO(sub)2 catalysts in photocatalytic oxidation of organic pollutants under visible light
Abstract:
Pollution of fresh water poses a problem that has been present since the beginning of Industrial Revolution. Organisation of United Nations estimates that there are currently over one billion people in the world without access to fresh drinking water. A problem unto itself are persistent pollutants which are used in large quantities in various branches of industry. Most notable endocrine-disrupting chemicals that fall into this category are bisphenols, which are known to have a strong effect on physiological processes even in relatively small quantities. In the last years, advanced oxidation processes have emerged as a novel way of removing persistent pollutants from wastewater. A wide array of advanced oxidation processes allows for a high degree of adjustment to the specifications set by the user in wastewater treatment. One of the most useful techniques in this regard is heterogenous photocatalysis in which photocatalitically active TiO2 is used as the catalyst. During the course of our experimental work, we prepared Au+TiO2 plasmonic catalysts. TiO2 nanoparticles were used as starting material in production of TiO2 nanorods with alkaline hydrothermal synthesis. Supported Au+TiO2 catalysts were produced from TiO2 nanorods and TiO2 nanoparticles in the process of deposition-precipitation. We evaluated physicochemical properties of Au+TiO2 catalysts and their photocatalytic performance upon irradiation with visible light. Furthermore, synthesized materials were used in photocatalytic oxidation reactions of four different bisphenols (bisphenol A, S, AF and F) under visible light. Concentrations of these pollutants during the experiment were monitored with the use of high performance liquid cromatography. Degrees of mineralization of organic pollutants were determined by measuring total organic carbon before and after experiments were conducted. Our research indicates that Au+TiO2 nanorods and Au+TiO2 nanoparticles differ in their physicochemical properties and in their photocatalytic performance under visible light. Presence of gold at the catalyst's surface has a significant impact on its catalytical performance under visible light. Our research also indicates that Au+TiO2 catalysts are suitable for use in degradation of organic pollutants such as bisphenols, although Au+TiO2 nanorods have proven to be a more effective catalyst than Au+TiO2 nanospheres in this regard. When using Au+TiO2 nanorods as the photocatalyst, 95 % of BPF, 80 % of BPA, slightly over 20 % of BPS and slightly under 20 % of BPAF were degraded during two hours of the reaction. Less successful degradation of the latter two pollutants can be attributed to their specific structural elements.

Keywords:Heterogenous photocatalysis, Au+TiO2 photocatalysts, advanced oxidation processes, endocrine-disrupting chemicals, bisphenols.

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