Comparative study of hydrogen evolution over perovskites and other oxides

Abstract

This study aims to compare the hydrogen evolution efficiency of photocatalysts based on titanate, tantalate, and niobium perovskite as well as some other oxides in 20% aqueous solution of various sacrificial agent. The solid-state reaction (SSR) method was used to prepare perovskites while nanopowder TiO2, Ta2O5 and Nb2O5 were used directly as purchased. 1 wt.% Pt cocatalyst was loaded on the samples by the incipient-to-wetness impregnation method; 0.2 wt.% Au, 1 wt.% Cu and 0.2 wt.% Au-0.8 wt.% Cu cocatalysts were also tested by loading them over TiO2 via deposition precipitation with urea (DPU) and sequential-DPU (S-DPU) methods. The hydrogen production rate on Pt/SrTiO3 under UV-VIS irradiation was much higher in D(+)-glucose monohydrate (GLU) (136.2 μmol/h.gcat), methanol (MeOH) (107.2 μmol/h.gcat), and ethylene glycol (EG) (112.5 μmol/h.gcat) solutions but it decreased after a maximum. However, the hydrogen generation rate in formic acid (FA) (54.8 μmol/h.gcat) and glycerol (GLY) (14.6 μmol/h.gcat) solutions were more stable. Pt/TiO2 was also tested in GLY solution, and the hydrogen production rate was found as 1146 μmol/h.gcat indicating a better potential than SrTiO3. 0.2 wt.% Au/TiO2 catalyst also produced 1085.1 μmol/h.gcat hydrogen even though Au loading is five times lower than Pt; furthermore, this catalyst also resulted in 201.4 μmol/h.gcat hydrogen, which is still significant and much higher than Pt under visible light irradiation. The distribution and size of shiny spherical gold particles around 40-50 nm size on TiO2 was observed by the scanning electron microscope (SEM) while the band gap energies were determined around 2.97 eV, which is quite close to TiO2, using UV-VIS spectroscopy by Kubelka-Munk method. X-ray diffraction (XRD) showed that mainly anatase phase exists in nanopowder TiO2 while SrTiO3 was mainly in the cubic crystal phase.