TY - JOUR
T1 - Efficient approach for simultaneous CO and H2 production via photoreduction of CO2 with water over copper nanoparticles loaded TiO2
AU - Singhal, Nikita
AU - Ali, Asgar
AU - Vorontsov, Alexander
AU - Pendem, Chandrashekar
AU - Kumar, Umesh
N1 - Publisher Copyright:
© 2016 Published by ElsevierB.V. All rights reserved.
PY - 2016/8/5
Y1 - 2016/8/5
N2 - Photoreduction of CO2 with water to alternative fuels using low cost meterials is an efficient approach to mitigate CO2. The present work describes a series of copper nanoparticles (Cu-NPs) loaded on TiO2, here copper nanoparticles were separately prepared by chemical reduction method, and then loaded on freshly synthesized TiO2. Oxidized and reduced forms of Cu/TiO2 nanoparticles were obtained by calcination under air and H2 respectively. Prepared catalysts were characterized by XRD, SEM, EDX, HR-TEM, XPS, BET surface area analysis, TPR, UV-vis diffuse reflectance spectroscopy and spectrofluorometry. Catalytic potential of prepared catalysts was checked for photocatalytic reduction of CO2 with water vapor under UV-C irradiation. The effect of oxidation state and loading amount of Cu as well as irradiation wavelength was also investigated. CO and H2 were observed as photocatalytic products. Among all the photocatalysts, 1% Cu-Red/TiO2 exhibited the highest photoactivity, with an initial rate of CO and H2 production of 334 and 452 μmol g-1 h-1 respectively, under UV-C light. The photocatalytic role of the Cu-NPs surface giving contribution to overall reaction was confirmed by using Cu-NPs, 1% Cu-Oxi/SiO2 and 1% Cu-Red/SiO2. A plausible mechanism of CO2 reduction is suggested and computationally confirmed. Reaction mechanism includes stages of CO2 adsorption at the Cu-TiO2 interface, reduction into HCO2, and dissociation into adsorbed hydroxyls and CO. The most energy demanding step was found to be CO desorption that could be facilitated by 254 nm quanta.
AB - Photoreduction of CO2 with water to alternative fuels using low cost meterials is an efficient approach to mitigate CO2. The present work describes a series of copper nanoparticles (Cu-NPs) loaded on TiO2, here copper nanoparticles were separately prepared by chemical reduction method, and then loaded on freshly synthesized TiO2. Oxidized and reduced forms of Cu/TiO2 nanoparticles were obtained by calcination under air and H2 respectively. Prepared catalysts were characterized by XRD, SEM, EDX, HR-TEM, XPS, BET surface area analysis, TPR, UV-vis diffuse reflectance spectroscopy and spectrofluorometry. Catalytic potential of prepared catalysts was checked for photocatalytic reduction of CO2 with water vapor under UV-C irradiation. The effect of oxidation state and loading amount of Cu as well as irradiation wavelength was also investigated. CO and H2 were observed as photocatalytic products. Among all the photocatalysts, 1% Cu-Red/TiO2 exhibited the highest photoactivity, with an initial rate of CO and H2 production of 334 and 452 μmol g-1 h-1 respectively, under UV-C light. The photocatalytic role of the Cu-NPs surface giving contribution to overall reaction was confirmed by using Cu-NPs, 1% Cu-Oxi/SiO2 and 1% Cu-Red/SiO2. A plausible mechanism of CO2 reduction is suggested and computationally confirmed. Reaction mechanism includes stages of CO2 adsorption at the Cu-TiO2 interface, reduction into HCO2, and dissociation into adsorbed hydroxyls and CO. The most energy demanding step was found to be CO desorption that could be facilitated by 254 nm quanta.
KW - CO and H production
KW - CO photoreduction
KW - Clusters
KW - Copper nanoparticles
KW - Cu/TiO
KW - DFT
KW - PM6
KW - Photocatalyst
UR - http://www.scopus.com/inward/record.url?scp=84974710193&partnerID=8YFLogxK
U2 - 10.1016/j.apcata.2016.05.027
DO - 10.1016/j.apcata.2016.05.027
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AN - SCOPUS:84974710193
SN - 0926-860X
VL - 523
SP - 107
EP - 117
JO - Applied Catalysis A: General
JF - Applied Catalysis A: General
ER -