Solar-assisted CO conversion into fuels and chemical products involves a range of technologies aimed at driving industrial decarbonization methods. In this work, we report on the development of a series of multifunctional metal-organic frameworks (MOFs) based on nitro- or amino-functionalized UiO-66(M) (M: Zr or Zr/Ti) supported RuO NPs as photocatalysts, having different energy band level diagrams, for CO hydrogenation under simulated concentrated sunlight irradiation. RuO(1 wt %; 2.2 ± 0.9 nm)@UiO-66(Zr/Ti)-NO was found to be a reusable photocatalyst, to be selective for CO methanation (5.03 mmol g after 22 h;, apparent quantum yield at 350, 400, and 600 nm of 1.67, 0.25, and 0.01%, respectively), and to show about 3-6 times activity compared with previous investigations. The photocatalysts were characterized by advanced spectroscopic techniques like femto- and nanosecond transient absorption, spin electron resonance, and photoluminescence spectroscopies together with (photo)electrochemical measurements. The photocatalytic CO methanation mechanism was assessed by operando FTIR spectroscopy. The results indicate that the most active photocatalyst operates under a dual photochemical and photothermal mechanism. This investigation shows the potential of multifunctional MOFs as photocatalysts for solar-driven CO recycling.
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| http://dx.doi.org/10.1021/acscatal.4c00266 | DOI Listing |
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