A "green" two-step methodology to prepare biobased gold-chitosan nanocomposite films using chitosan and AuCl as a stabilizer and precursor, respectively, is reported. The biobased nanocomposites were prepared in situ by a wet chemical reduction method. Effects of hydrazine and l-ascorbic acid as different strength reducing agents on the characteristics of gold nanoparticles were observed. In addition, the performance of these nanocomposite films as catalytic materials was assessed. The relevance of this work underlies that the catalytic activity, conversion degree and order of the reaction of the 4-nitrophenol-sodium borohydride (4NP-NaBH) reduction system depend on the size distribution, content and mainly to the location of gold nanoparticles in the nanocomposite films. Finally, the potential recyclability of these nanocomposite films as catalytic materials was studied.
Fourth generation polyamidoamine dendrimer (PAMAM, G4) modified with fluorescein units (F) at the periphery and Pt nanoparticles stabilized by L-ascorbate were prepared. These dendrimers modified with hydrophobic fluorescein were used to achieve self-assembling structures, giving rise to the formation of nanoaggregates in water. The photoactive fluorescein units were mainly used as photosensitizer units in the process of the catalytic photoreduction of water propitiated by light. Complementarily, Pt-ascorbate nanoparticles acted as the active sites to generate H2. Importantly, the study of the functional, optical, surface potential and morphological properties of the photosensitized dendrimer aggregates at different irradiation times allowed for insights to be gained into the behavior of these systems. Thus, the resultant photosensitized PAMAM-fluorescein (G4-F) nanoaggregates (NG) were conveniently applied to light-driven water photoreduction along with sodium L-ascorbate and methyl viologen as the sacrificial reagent and electron relay agent, respectively. Notably, these aggregates exhibited appropriate stability and catalytic activity over time for hydrogen production. Additionally, in order to propose a potential use of these types of systems, the in situ generated H2 was able to reduce a certain amount of methylene blue (MB). Finally, theoretical electronic analyses provided insights into the possible excited states of the fluorescein molecules that could intervene in the global mechanism of H2 generation.
The synthesis and the electrochemical, photoluminescent and electroluminescent properties is reported for two new Ir(iii) cyclometalated complexes described as [Ir(F2ppy)2L1](PF6) and [Ir(F2ppy)2L2](PF6).
Biobased tractable films consisting of blends of chitosan (CS) with polymer bearing carbazole derivatives as pendant groups and fluorene-thiophene as donor-acceptor units (referred to as DA) were prepared, and their optical, morphological and photocatalytic properties were studied. DA was dissolved in tetrahydrofuran (THF) and mixed with an acidified aqueous solution containing chitosan to obtain chitosan/DA (CS/DA) films by solution casting. The fabricated biobased films were characterized using spectroscopic techniques (FT-IR and UV-vis), thermogravimetry, mechanical assays, contact angle analysis, and atomic force microscopy (AFM). The effects of varying DA compositions and the results of exposure to visible-light irradiation of the films were also analyzed. The results indicated the existence of interactions between chitosan and DA and a potentially profitable light-driven response of these biobased films. This behavior was reflected in the optical, topographical, and contact angle properties of the films, which exhibited different characteristics before and after visible-light exposure. Finally, the photocatalytic performance of the biobased films was tested via the decomposition of methyl orange (MO), as a reaction model system. Our results revealed a significant photocatalytic activity (according to biobased film composition, approximately 64 % and 87 % of methyl orange were degraded under continuous visible-light irradiation for 120 min) of the films which is attributed to the combined presence and synergetic effects of the film-forming ability of chitosan and the photoproperties of DA.
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