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Keywords: polyacetylenes, emulsion-templating, π-conjugated networks, macroporous polymers, heterogeneous photocatalysis
Published in DKUM: 29.08.2024; Views: 73; Downloads: 3
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Abstract: Highly porous metal oxide−polymer nanocomposites are attracting considerable interest due to their unique structural and functional features. A porous polymer matrix brings properties such as high porosity and permeability, while the metal oxide phase adds functionality. For the metal oxide phase to perform its function, it must be fully accessible, and this is possible only at the pore surface, but functioning surfaces require controlled engineering, which remains a challenge. Here, highly porous nanocomposite beads based on thin metal oxide nanocoatings and polymerized high internal phase emulsions (polyHIPEs) are demonstrated. By leveraging the unique properties of polyHIPEs, i.e., a three-dimensional (3D) interconnected network of macropores, and high-precision of the atomic-layer-deposition technique (ALD), we were able to homogeneously coat the entire surface of the pores in polyHIPE beads with TiO$_2$-, ZnO-, and Al$_2$O$_3$-based nanocoatings. Parameters such as nanocoating thickness, growth per cycle (GPC), and metal oxide (MO) composition were systematically controlled by varying the number of deposition cycles and dosing time under specific process conditions. The combination of polyHIPE structure and ALD technique proved advantageous, as MO-nanocoatings with thicknesses between 11 ± 3 and 40 ± 9 nm for TiO$_2$ or 31 ± 6 and 74 ± 28 nm for ZnO and Al$_2$O$_3$, respectively, were successfully fabricated. It has been shown that the number of ALD cycles affects both the thickness and crystallinity of the MO nanocoatings. Finally, the potential of ALD-derived TiO$_2$-polyHIPE beads in photocatalytic oxidation of an aqueous bisphenol A (BPA) solution was demonstrated. The beads exhibited about five times higher activity than nanocomposite beads prepared by the conventional (Pickering) method. Such ALD-derived polyHIPE nanocomposites could find wide application in nanotechnology, sensor development, or catalysis.
Keywords: nanovlakna, aerosoli, filtracija, emulsion-templating, macroporous polymers, atomic-layer-deposition
Published in DKUM: 15.04.2024; Views: 249; Downloads: 17
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Abstract: Access to conjugated porous polymers via synthetically sustainable and straightforward routes is highly desirable, as many polymer systems exhibit high performance but require arduous synthetic protocols that rarely pave the way to commercial reality. In this article, we describe an easily fabricated series of novel highly porous poly(Schiff bases) that feature an aliphatic conjugated backbone obtained with low synthetic complexity from simple reagents such as glyoxal and hydrazine monohydrate in water. The effective synthesis enables the preparation of three different functional scaffolds, i.e., aerogels, polyHIPEs (polymerized HIPEs), and even carbon foams from aliphatic poly(azine) (PAZ) networks. The reported synthetic approach is compared to the literature using ″green chemistry metrics″, such as the E-factor and synthetic complexity (SC) index, and shows dramatic improvements. An E-factor of up to 0.27 for aerogels or 80 for polyHIPEs and an SC index of 2.7 are much lower than those for poly(arylene)-based conjugated analogues, indicating good scalability, sustainability, and low cost. PAZ materials feature impressive red/near IR-shifted optical absorption band edges, with an electrochemical band gap of 1.45 eV. Aliphatic PAZ scaffolds are characterized by high flexibility compared to aromatic analogues and do not fail at compressive loads of up to 70%. Finally, carbonization at 500 °C leads to highly porous carbonaceous scaffolds with a high N content of up to 29 wt % (21 mmol of nitrogen per gram carbon material).
Published in DKUM: 13.03.2024; Views: 696; Downloads: 17
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Keywords: analizna kemija, organske snovi, organska analiza, učbeniki
Published in DKUM: 19.09.2023; Views: 825; Downloads: 35
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Abstract: Vse večji in naprednejši razvoj industrije ter kmetijstva vzporedno z rastjo populacije povzroča ogromno škodo okolju z izpustom škodljivih kemikalij in ostalih organskih onesnaževal. Večina teh polutantov je toksičnih, mutagenih in karcinogenih, ki so zelo obstojni ter se zlahka bioakumulirajo. V to kategorijo sodijo tudi motilci endokrinega sistema (bisfenol A) z močnim vplivom na fiziološke procese v človeškem organizmu in zaskrbljujoča nova onesnaževala (farmacevtske učinkovine) z znanimi ali domnevnimi učinki na okolje ter zdravje človeka. V odgovor ekološki zaskrbljenosti zaradi obsežnega onesnaževanja pitne vode, rek, jezer in morja, se je v zadnjih desetletjih med znanstveniki povečalo zanimanje za razvoj novih tehnologij na področju čiščenja odpadnih voda. Velik potencial pri učinkovitem odstranjevanju organskih onesnaževal iz vodnih sistemov so pokazali napredni oksidacijski procesi, ki s prilagajanjem postopkov oksidacije dosežejo neselektivno razgradnjo organskih snovi do CO2 in vode. Med temi procesi velja metoda heterogene fotokatalize z uporabo fotokatalizatorjev na osnovi TiO2 za najbolj raziskano, obetavno, enostavno in okolju prijazno. Namen magistrske naloge je bil z metodo mokre impregnacije pripraviti fotokatalizatorje na osnovi TiO2 nanodelcev, ki bodo uspešno razgradili organska onesnaževala v šaržnem reaktorju ob obsevanju z vidno svetlobo. Ker je čisti TiO2 aktiven samo v ultravijoličnem spektru svetlobe, smo na njegovo površino dopirali plazmonski žlahtni kovini (Au, Pt) in njune zlitine. S karakterističnimi metodami smo sintetiziranim katalizatorjem določili njihove optične, strukturne in površinske lastnosti ter preverili učinkovitost pri tvorjenju reaktivnih kisikovih zvrsti (HO• s kumarinom ter O2•- in e- z ABTS•+). Fotokatalitsko aktivnost pri razgradnji bisfenola A pod svetlobo v vidnem delu spektra smo ugotovili s tekočinsko kromatografijo visoke ločljivosti in z merjenjem celotnega organskega ogljika pred in po fotokatalizi določili stopnjo mineralizacije onesnaževal. Sintetizirani fotokatalizatorji so se med seboj razlikovali v optičnih in površinskih lastnostih, po učinkovitosti tvorbe reakcijskih kisikovih zvrsti ter razgradnje bisfenola A. Ugotovili smo tudi, da nanos Au, Pt in njunih zlitin na površino nosilca TiO2 ne vpliva na njegovo morfologijo. Pri razgradnji bisfenola A je bil najbolj učinkovit fotokatalizator z nanosom zlitine 0,25 % Au + 0,75 % Pt (80,7 %), sledil mu je katalizator z nanosom zlitne 0,5 % Au + 0,5 % Pt (74,5 %), še sprejemljivo razgradnjo pa je dosegel katalizator z nanosom 1 % Pt (70,9 %). Ker je katalizator z dopirano zlitino 0,5 % Au + 0,5 % Pt teoretično izkazoval potencialno veliko katalitsko aktivnost, smo ga uporabili še za preverjanje učinkovitosti razgradnje farmacevtskih učinkovin, kot so aspirin, kofein in paracetamol. Izbrani katalizator je bil najbolj uspešen pri razgradnji aspirina (97 %), naslednji je bil kofein (79 %), paracetamola pa se je razgradilo nekoliko majn (62 %). Zbrani podatki so potrdili fotokatalitski potencial katalizatorjev z dopiranimi zlitinami Au in Pt, kjer ima Pt prevladujoč ali enak deleže od Au pri razgradnji bisfenola A in farmacevtskih učinkovin (aspirin, kofein in paracetamol).
Keywords: napredni oksidacijski procesi, heterogena fotokataliza, TiO2 fotokatalizatorji, žlahtni kovini Au in Pt, fotokataliza pod vidno svetlobo, organska onesnaževala
Published in DKUM: 13.09.2023; Views: 400; Downloads: 60
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