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Photocatalytic water splitting by N-TiO₂ on MgO (111) with exceptional quantum efficiencies at elevated temperatures.

ABSTRACT: Photocatalytic water splitting is attracting enormous interest for the storage of solar energy but no practical method has yet been identified. In the past decades, various systems have been developed but most of them suffer from low activities, a narrow range of absorption and poor quantum efficiencies (Q.E.) due to fast recombination of charge carriers. Here we report a dramatic suppression of electron-hole pair recombination on the surface of N-doped TiO₂ based nanocatalysts under enhanced concentrations of H⁺ and OH^-, and local electric field polarization of a MgO (111) support during photolysis of water at elevated temperatures. Thus, a broad optical absorption is seen, producing O₂ and H₂ in a 1:2 molar ratio with a H₂ evolution rate of over 11,000 μmol g^-1 h^-1 without any sacrificial reagents at 270 °C. An exceptional range of Q.E. from 81.8% at 437 nm to 3.2% at 1000 nm is also reported.

SUBMITTER: Li Y

PROVIDER: S-EPMC6764948 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Titanium dioxide (TiO2) in the form of thin films has attracted enormous attention for photocatalysis. It combines the fundamental properties of TiO2 as a large bandgap semiconductor with the advantage of thin films, making it competitive with TiO2 powders for recycling and maintenance in photocatalytic applications. There are many aspects affecting the photocatalytic performance of thin film structures, such as the nanocrystalline size, surface morphology, and phase composition. However, the quantification of each influencing aspect needs to be better studied and correlated. Here, we prepared a series of TiO2 thin films using a sol-gel process and spin-coated on p-type, (100)-oriented silicon substrates with a native oxide layer. The as-deposited TiO2 thin films were then annealed at different temperatures from 400 °C to 800 °C for 3 h in an ambient atmosphere. This sample synthesis provided systemic parameter variation regarding the aspects mentioned above. To characterize thin films, several techniques were used. Spectroscopic ellipsometry (SE) was employed for the investigation of the film thickness and the optical properties. The results revealed that an increasing annealing temperature reduced the film thickness with an increase in the refractive index. Atomic force microscopy (AFM) was utilized to examine the surface morphology, revealing an increased surface roughness and grain sizes. X-ray diffractometry (XRD) and UV-Raman spectroscopy were used to study the phase composition and crystallite size. The annealing process initially led to the formation of pure anatase, followed by a transformation from anatase to rutile as the annealing temperature increased. An overall enhancement in crystallinity was also observed. The photocatalytic properties of the thin films were tested using the photocatalytic decomposition of acetone gas in a home-built solid (photocatalyst)-gas (reactant) reactor. The composition of the gas mixture in the reaction chamber was monitored using in situ Fourier transform infrared spectroscopy. Finally, all of the structural and spectroscopic characteristics of the TiO2 thin films were quantified and correlated with their photocatalytic properties using a correlation matrix. This provided a good overview of which film properties affect the photocatalytic efficiency the most.

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Photocatalytic water splitting by N-TiO₂ on MgO (111) with exceptional quantum efficiencies at elevated temperatures.

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Dataset Information

Photocatalytic water splitting by N-TiO2 on MgO (111) with exceptional quantum efficiencies at elevated temperatures.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

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Photocatalytic water splitting by N-TiO₂ on MgO (111) with exceptional quantum efficiencies at elevated temperatures.