Intensifying CO2 photoreduction into value-added fuels using microscale illumination

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Solar thermo-photocatalytic methanation using a bifunctional RuO2:TiO2/Z13X photocatalyst/adsorbent material for efficient CO2 capture and conversion

Publication . Paulista, Larissa O.; Ferreira, Alexandre F.P.; Rodrigues, Alírio; Martins, Ramiro; Boaventura, Rui; Vilar, Vítor J.P.; Silva, Tânia F.C.V.

A novel bifunctional photocatalyst/adsorbent material based on the RuO2:TiO2/zeolite 13X (Z13X) composite was developed to enhance solar-driven methanation through simultaneous carbon dioxide (CO2) capture and thermo-photoconversion. The activity/stability of the hybrid material towards methane (CH4) production was assessed by varying the (i) photocatalyst composition (Ru load and semiconductor type), (ii) bifunctional material composition (photocatalyst-to-zeolite ratio) and impregnation method, (iii) illumination source and power (simulated sunlight and UVA/Visible LEDs), (iv) temperature, and (v) catalyst reuse. Additionally, adsorption equilibrium isotherms were determined to characterize the adsorption ability of the bifunctional material for both CO2 and CH4 gases. The hybrid RuO2(4.0%):TiO2(26.3%)/Z13X material (30 mg), synthesised by the solid-state impregnation method, showed the best results under simulated sunlight (0.75 W) at 150 ºC, achieving a 88% CO2 thermo-photoreduction after 100 min, corresponding to a specific CH4 production of 29.2 mmol gactive_cat−1 h−1 (309 mmol gRu−1 h−1) and apparent quantum yield of 20.7%. In adsorption equilibrium isotherms, the bifunctional material's adsorption was about 2.6-fold higher than the photocatalyst at 150 ºC, suggesting that enhanced methanation performance can be attributed to the synergistic action of CO2 capture and thermo-photoconversion.

2024Journal article

Open access

Solar-driven thermo-photocatalytic CO2 methanation over a structured RuO2:TiO2/SBA-15 nanocomposite at low temperature

Publication . Paulista, Larissa Oliveira; Ferreira, Alexandre; Castanheira, Bruna; Ðolić, Maja B.; Martins, Ramiro; Boaventura, Rui; Vilar, Vítor J.P.; Silva, Tânia F.C.V.

A new hybrid catalyst composed of mesostructured silica SBA-15 functionalized with TiO2 and further loaded with RuO2 was developed to efficiently promote thermo-photocatalytic CO2 hydrogenation into methane at low temperatures. The catalytic activity was assessed with respect to TiO2:RuO2 loading, catalyst dosage, illumination source (polychromatic sunlight and monochromatic LEDs) and power, [H2]:[CO2] molar ratio, temperature, and catalyst reusability. The best methanation yields were attained for the RuO2(6.4%):TiO2(16.9%)/SBA-15 nanocomposite at 150 ºC, under simulated sunlight (0.21 W) and stoichiometric [H2]:[CO2] molar ratio, reaching: a specific CH4 production rate of 13.6 mmol g-c1a t h-1; 99.8 % selectivity; 96.8 % CO2 conversion (110- min; 40 mL); and apparent photonic efficiency/quantum yield of 39.5 %/42.1 %. Considering only the active RuO2:TiO2 photocatalyst mass (23.3 %), the CH4 production rate increased to 58.6 mmol g-a1c tive_cat h-1. Besides, this highly-active photocatalyst featured excellent UV-Vis-IR light absorbance, high surface area, and stability for reuse when moist gas was removed between cycles.

2024Journal article

Open access