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

abstract

  • 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.
  • This work was financially supported by: (i) LA/P/0045/2020 (ALiCE), UIDB/50020/2020 and UIDP/50020/2020 (LSRE-LCM), funded by national funds through Fundação para a Ciência e a Tecnologia (FCT), and Ministério da Ciência, Tecnologia e Ensino Superior (MCTES), Portugal, under Programa de Investimento e Despesas de Desenvolvimento da Administração Central (PIDDAC); (ii) project HyGreen&LowEmissions (NORTE-01-0145-FEDER-000077), supported by Norte Portugal Regional Operational Programme (NORTE 2020), under the PORTUGAL 2020 Partnership Agreement, through the European Regional Development Fund (ERDF); and (iii) project CO2-to-CH4 (2022.01176. PTDC), supported by national funds through the FCT/MCTES (PIDDAC). Larissa O. Paulista acknowledges the Ph.D. fellowship supported by FCT (reference SFRH/BD/137639/2018 and COVID/BD/152922/2022). Maja B. Đolíc acknowledges the Ministry of Education, Science and Technological Development of the Republic of Serbia (Contract No. 451–03-9/2022–14/200135). Tˆania F.C.V. Silva acknowledges the FCT Individual Call to Scientific Employment Stimulus 2017 (CEECIND/ 01386/2017).

publication date

  • January 1, 2024