TiO2 thin films with different titanium isopropoxide (TTIP):acetylacetone (AcacH) molar ratios in solution were prepared by the chemical spray pyrolysis method. The TTIP:AcacH molar ratio in spray solution varied from 1:3 to 1:20. TiO2 films were deposited onto the glass substrates at 350 °C and heat-treated at 500 °C. The morphology, structure, surface chemical composition, and photocatalytic activity of the obtained TiO2 films were investigated. TiO2 films showed a transparency of ca 80% in the visible spectral region and a band gap of ca 3.4 eV irrespective of the TTIP:AcacH molar ratio in the spray solution. TiO2 films consist of the anatase crystalline phase with a mean crystallite size in the range of 30–40 nm. Self-cleaning properties of the films were estimated using the stearic acid (SA) test. A thin layer of 8.8-mM SA solution was spin-coated onto the TiO2 film. The degradation rate of SA as a function of irradiation time was monitored by Fourier-transform infrared spectroscopy (FTIR). An increase in the TTIP:AcacH molar ratio from 1:4 to 1:8 resulted in a ten-fold increase in the photodegradation reaction rate constant (from 0.02 to the 0.2 min−1) under ultraviolet light and in a four-fold increase under visible light.
Enhanced photocatalytic oxidation of indoor VOC mixtures on transparent polycrystalline spray-deposited TiO2 thin films under ultraviolet and visible light.
13 September 2022 in ACS Applied Materials & Interfaces
For the efficient photocatalytic oxidation of organic pollutants at surfaces of semiconductors, photogenerated holes shall be separated toward the surface and transferred to reactive surface sites, whereas the transfer of photogenerated electrons toward the surface shall be minimized. In this Research Article, the identification of suitable synthesis control of charge separation combined with an in-depth understanding of charge kinetics and trapping passivation mechanisms at the related surfaces can provide tremendous opportunities for boosting the photocatalytic performance. In this work, a comprehensive transient surface photovoltage spectroscopy study of charge separation at anatase TiO2 thin films, synthesized by ultrasonic spray pyrolysis from titanium(IV) isopropoxide (TTIP)-acetylacetone (AcacH) based precursor is reported. By varying the amount of AcacH in the precursor solution, an experimental approach of synthesis control of the charge transfer toward TiO2 surface is provided for the first time. An increased amount of AcacH in the precursor promotes transition from preferential fast electron to preferential fast hole transfer toward anatase surface, correlating with a strong increase of the photocatalytic decomposition rate of organic pollutants. Suitable mechanisms of AcacH-induced passivation of electron traps at TiO2 surfaces are analyzed, providing a new degree of freedom for tailoring the properties of photocatalytic systems.
TiO2 thin films, modified by acetylacetone (AcacH) in solution, were deposited on glass substrate by ultrasonic spray pyrolysis and tested for photocatalytic activity in a multi-section continuous flow reactor by degradation of acetone and acetaldehyde under ultraviolet and visible light. The increase in molar ratio of AcacH in respect of titanium (IV) isopropoxide (TTIP) from 1:5 to 1:8 modified the electronic structure of the films, favoring enhanced photocatalytic activity. The photocatalytic activity was enhanced approximately twofold on the film with molar ratio 1:8 under both irradiations; the film completely oxidized 10 ppm of acetone and acetaldehyde. The photocatalytic efficacy of TiO2 films in oxidation of air pollutants was three times higher compared to the industrial glass Pilkington ActivTM. Moreover, all the synthesized films indicate antibacterial efficiency against E. coli of over 99% under ultraviolet. TiO2 film, with TTIP:AcacH molar ratio 1:8 having great possibility for its commercial use as a material for indoor air purification.
The synthesis of TiO2 thin films by the chemical spray pyrolysis method at different titanium isopropoxide (TTIP) to acetylacetone (AcacH) ratios has been shown to lead to the highest photodegradation at 1 (TTIP):8 (AcacH). These films hold promise in the field of indoor pollution treatment. Carbon incorporation into the surface and into the TiO2 lattice could be responsible for the observed performance, but the mechanism is still to be elucidated. Here, we report the correlation of contact potential difference (CPD) contrast maps as produced using Kelvin Probe Force Microscopy, and the observed functionality dependence on the TTIP to AcacH ratio. Since the CPD contrast locally provides information about the sample's Fermi level, this correlation provides a means to interpret enhanced photocatalytic activity in terms of the presence of acceptors that make possible a faster transfer of charge carriers to the surface.