Proceedings of Catalyst Design Strategies for Photo- and Electrochemical Fuel Synthesis (ECAT25)
Publication date: 19th December 2024
Photothermal catalysis may provide highly efficient conversion of CO2 to value-added products. Here, both the principles of heterogeneous photocatalysis and ‘classic’ thermocatalysis are combined to achieve high reaction rates and to possibly open up new chemical pathways [1-3]. Photothermal catalysis can be realized by depositing specific metal nanoparticles on a support material, typically a semiconductor. Such nanoparticles can absorb a broad part of the solar spectrum, including visible light. As a result, plasmonic or non-plasmonic effects will result in the conversion of the absorbed photon energy in high energetic charge carriers. These charge carriers are either injected into the photocatalytic particle, or they thermalize and thereby release localized heat to the environment. This causes an increase in (photo)catalytic performance of the photothermal system. To enhance the activity even further, external heating can be used as well.
In this study, we demonstrate that we can successfully photothermally convert CO2 and H2 into CH4 (i.e., the Sabatier reaction) using Ru/TiO2 catalysts, where Ru nanoparticles are deposited on a TiO2 support. By raising the external temperature mildly, we see a significant increase in light sensitivity of the particles, with the effect being strongest in the range of 180 – 200 oC. A further increase in temperature yields a shift in selectivity towards CO production. Interestingly, we see photothermal activity not only under UV-vis illumination, but also clearly under visible light illumination. To understand the photophysics, we performed time-resolved photoluminescence (PL) spectroscopy experiments [4]. We studied the behavior and migration of charge carriers within the system when either the TiO2 is dominantly photoexcited by 267 nm, or when the Ru is dominantly photoexcited by 532 nm visible light. Additionally, we performed diffuse reflectance infrared Fourier Transform (DRIFT) spectroscopy studies to understand the surface chemistry taking place during the photothermal methanization of CO2. Based on our findings, we propose a model how these physical and chemical aspects are connected in the photothermal methanization of CO2 using Ru/TiO2 nanostructures. We will also discuss strategies how these insights can be used to modify these structures to yield even higher activities and selectivities.
We would like to acknowledge Prof. Dr. Niemantsverdriet and Dr. Fredriksson of SynGasChem BV for their useful discussions and their financial support. Furthermore, we would like to thank the Dutch Science Foundation (NWO) for funding as a part of the solar to products project Solar to Products Program 733.000.001. Furthermore, we like to thank the Dutch Ministry of Education, Culture and Science for their financial support in the form of a Starter Grant.
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