Turning Carbon Dioxide And Ethane Into Ethanol By Solar-Driven Heterogeneous Photocatalysis Over Ruo2- And Nio-Co-Doped Srtio3

CATALYSTS(2021)

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摘要
The current work focused on the sunlight-driven thermo-photocatalytic reduction of carbon dioxide (CO2), the primary greenhouse gas, by ethane (C2H6), the second most abundant element in shale gas, aiming at the generation of ethanol (EtOH), a renewable fuel. To promote this process, a hybrid catalyst was prepared and properly characterized, comprising of strontium titanate (SrTiO3) co-doped with ruthenium oxide (RuO2) and nickel oxide (NiO). The photocatalytic activity towards EtOH production was assessed in batch-mode and at gas-phase, under the influence of different conditions: (i) dopant loading; (ii) temperature; (iii) optical radiation wavelength; (vi) consecutive uses; and (v) electron scavenger addition. From the results here obtained, it was found that: (i) the functionalization of the SrTiO3 with RuO2 and NiO allows the visible light harvest and narrows the band gap energy (ca. 14-20%); (ii) the selectivity towards EtOH depends on the presence of Ni and irradiation; (iii) the catalyst photoresponse is mainly due to the visible photons; (iv) the photocatalyst loses > 50% efficiency right after the 2nd use; (v) the reaction mechanism is based on the photogenerated electron-hole pair charge separation; and (vi) a maximum yield of 64 mu mol EtOH g(cat)(-1) was obtained after 45-min (85 mu mol EtOH g(cat)(-1) h(-1)) of simulated solar irradiation (1000 W m(-2)) at 200 degrees C, using 0.4 g L-1 of SrTiO3:RuO2:NiO (0.8 wt.% Ru) with [CO2]:[C2H6] and [Ru]:[Ni] molar ratios of 1:3 and 1:1, respectively. Notwithstanding, despite its exploratory nature, this study offers an alternative route to solar fuels' synthesis from the underutilized C2H6 and CO2.
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关键词
heterogeneous thermo-photocatalysis, solar fuels synthesis, hybrid perovskite catalyst, double doping approach, CO2 photoconversion, ethane upgrading
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