A facile development of highly efficient Pt-TiO(2) nanostructured films via versatile gas-phase deposition methods is described. The films have a unique one-dimensional (1D) structure of TiO(2) single crystals coated with ultrafine Pt nanoparticles (NPs, 0.5-2 nm) and exhibit extremely high CO(2) photoreduction efficiency with selective formation of methane (the maximum CH(4) yield of 1361 μmol/g-cat/h). The fast electron-transfer rate in TiO(2) single crystals and the efficient electron-hole separation by the Pt NPs were the main reasons attributable for the enhancement, where the size of the Pt NPs and the unique 1D structure of TiO(2) single crystals played an important role.
An aerosol-chemical vapor deposition (ACVD) was designed to deposit nanostructured metal oxide films with controlled morphologies. Characteristic times of the different processes governing deposition of the film were used to establish the relationship of process parameters to the resultant morphology of the film. Titanium dioxide (TiO2) films were synthesized with different morphologies: dense, columnar, granular, and branched tree-type structures. The developed ACVD process was also used to deposit columnar nickel oxide (NiO) films. The various films with well-controlled characteristics (length, morphology) were used to establish the performance in solar energy applications, such as photosplitting of water to produce hydrogen. Columnar TiO2 films of 1.6 μm length with a platinum wire counter electrode resulted in 15.58% hydrogen production efficiencies under UV light illumination, which was 2.50 times higher than dense TiO2 films with a platinum wire counter electrode. On replacing the Pt counter electrode with a columnar NiO film, efficiencies of 10.98% were obtained.
Two novel deposition methods were used to synthesize Pt-TiO(2) composite photoelectrodes: a tilt-target room temperature sputtering method and aerosol-chemical vapor deposition (ACVD). Pt nanoparticles (NPs) were sequentially deposited by the tilt-target room temperature sputtering method onto the as-synthesized nanostructured columnar TiO(2) films by ACVD. By varying the sputtering time of Pt deposition, the size of deposited Pt NPs on the TiO(2) film could be precisely controlled. The as-synthesized composite photoelectrodes with different sizes of Pt NPs were characterized by various methods, such as SEM, EDS, TEM, XRD, and UV-vis. The photocurrent measurements revealed that the modification of the TiO(2) surface with Pt NPs improved the photoelectrochemical properties of electrodes. Performance of the Pt-TiO(2) composite photoelectrodes with sparsely deposited 1.15 nm Pt NPs was compared to the pristine TiO(2) photoelectrode with higher saturated photocurrents (7.92 mA/cm(2) to 9.49 mA/cm(2)), enhanced photoconversion efficiency (16.2% to 21.2%), and increased fill factor (0.66 to 0.70). For larger size Pt NPs of 3.45 nm, the composite photoelectrode produced a lower photocurrent and reduced conversion efficiency compared to the pristine TiO(2) electrode. However, the surface modification by Pt NPs helped the composite electrode maintain higher fill factor values.
Energy issues are important and consumption is slated to increase across the globe in the future. The energy-environment nexus is very important as strategies to meet future energy demand are developed. To ensure sustainable growth and development, it is essential that energy production is environmentally benign. There are two temporal issues-one that is immediate, and needs to address the environmental compliance of energy generation from fossil fuel sources; and second that is the need to develop newer alternate and more sustainable approaches in the future. Aerosol science and technology is an enabling discipline that addresses the energy issue over both these time scales. The paper is a review of aspects of aerosol science and engineering that helps address carbon neutrality of fossil fuels. Advanced materials to meet these challenges are discussed. Future approaches to effective harvesting of sunlight that are enabled by aerosol studies are discussed.
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