TY - JOUR
T1 - Continuous flow gas phase photoreforming of methanol at elevated reaction temperatures sensitised by Pt/TiO2
AU - Caravaca, Angel
AU - Daly, Helen
AU - Smith, M
AU - Mills, Andrew
AU - Chansai, Sarayute
AU - Hardacre, Christopher
PY - 2017/3/31
Y1 - 2017/3/31
N2 - Gas phase photoreforming of methanol using a Pt/TiO2 photocatalyst has been performed
under flow conditions at elevated temperatures. Comparing the activity of the reforming
process as a function of temperature under dark and irradiated conditions shows a significant
enhancement in the rate of H2 production using the photo-assisted conditions at temperatures
between 100-140 °C. At higher temperatures, the effect of irradiation is small with the
process dominated by the thermal process. Deactivation of the catalyst was observed under
irradiation but the catalyst was easily regenerated using an oxygen treatment at 120 °C.
Diffuse Reflectance Infra-red Fourier Transform Spectroscopy (DRIFTS) showed that the
activity of the catalyst could be correlated with the presence of the photogenerated trapped
electrons. In addition, lower amounts of CO adsorbed on Pt, compared to those observed in
the dark reaction, were found for the UV-irradiated systems. It is proposed that CO and
adsorbed intermediates, such as formate, can act as inhibitors in the photoreforming process
and this is further supported by the observation that, before and after the regeneration process
in O2, the CO and surface adsorbed organic intermediate products are removed and the
activity is recovered.
AB - Gas phase photoreforming of methanol using a Pt/TiO2 photocatalyst has been performed
under flow conditions at elevated temperatures. Comparing the activity of the reforming
process as a function of temperature under dark and irradiated conditions shows a significant
enhancement in the rate of H2 production using the photo-assisted conditions at temperatures
between 100-140 °C. At higher temperatures, the effect of irradiation is small with the
process dominated by the thermal process. Deactivation of the catalyst was observed under
irradiation but the catalyst was easily regenerated using an oxygen treatment at 120 °C.
Diffuse Reflectance Infra-red Fourier Transform Spectroscopy (DRIFTS) showed that the
activity of the catalyst could be correlated with the presence of the photogenerated trapped
electrons. In addition, lower amounts of CO adsorbed on Pt, compared to those observed in
the dark reaction, were found for the UV-irradiated systems. It is proposed that CO and
adsorbed intermediates, such as formate, can act as inhibitors in the photoreforming process
and this is further supported by the observation that, before and after the regeneration process
in O2, the CO and surface adsorbed organic intermediate products are removed and the
activity is recovered.
U2 - 10.1039/C6RE00140H
DO - 10.1039/C6RE00140H
M3 - Article
VL - 1
SP - 649
EP - 657
JO - Reaction Chemistry & Engineering
JF - Reaction Chemistry & Engineering
SN - 2058-9883
ER -