Scaling-up a Photo-Electrocatalytic Reactor for CO2 Capture and Conversion to Syngas

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The most challenging deal we face today is the need to lower greenhouse gas (GHG) emissions and tackle climate change. Though calls to reduce them are growing louder yearly, emissions remain unsustainably high. CO2 is the key contributor to global climate change in the atmosphere. Electrochemical CO2 reduction (EC CO2R) into chemicals or fuels holds great research interest as a promising approach to mitigate CO2 emissions and reach a carbon-neutral future.1 In this regard, an extraordinary effort has been made to discover new efficient and sustainable catalysts at the laboratory level over recent years. High-performance electrocatalysts in aqueous electrolytes often rely on noble metals, which may hinder their industrial applications. Herein, we successfully synthesized core-shell Cu2O/SnO2 nanoparticles2–4 functionalized with a silane group, using a simple and versatile methodology based on a three-step scalable synthesis method involving wet precipitation followed by salinization and, finally, a rhenium-based complex has been assembled by electro-polymerization.5 The carbon paper-supported Cu2O/SnO2-Re electrocatalyst was characterized at 10 cm2 scale achieving a CO:H2 ratio from 3 to 9, and demonstrating an stable syngas production up to 24 hours at -20 mA·cm-2. To translate those developments from the laboratory level to a higher TRL towards the practical application of CO2 capture and utilization6, an additional chamber was added to the system for the continuous CO2 capture and electrochemical conversion, increasing the electrode area from 10 cm2 to 100 cm2. Captured CO2 co-electrolysis to syngas (H2:CO ratio of 5) in one step was demonstrated with a high CO2 conversion at a current up to -2 A, indicating the scale-up potential of this intensified system. The technology is currently under validation in a TRL4 reactor composed of an array of 5 modules (i.e., 4 x 5 cells x 100 cm2) with a total active area of or 0.2m2 for direct CO2 conversion from simulated anthropogenic sources. The design integrates low-cost photovoltaic (PV) cells to provide any required additional bias to drive the reaction, thus, Perovskite PV panels with a cost of up to 5 times lower (10 €/m2) than Si PV cells were used. The TRL5 demonstration of the developed technology will be done with real flue gas emissions the first semester of 2024. Acknowledgements The financial support of the SUNCOCHEM project (Grant Agreement No 862192) of the European Union’s Horizon 2020 Research and Innovation Action programme is acknowledged. References Guzmán, H., Russo, N. & Hernández, S. CO2 valorisation towards alcohols by Cu-based electrocatalysts: challenges and perspectives. Green Chemistry vol. 23 1896–1920 Preprint at https://doi.org/10.1039/d0gc03334k (2021).Cuatto, G. et al. Standardization of Cu2O nanocubes synthesis: Role of precipitation process parameters on physico-chemical and photo-electrocatalytic properties. Chemical Engineering Research and Design 199, 384–398 (2023).Zoli, M., Guzmán, H., Sacco, A., Russo, N. & Hernández, S. Cu2O/SnO2 Heterostructures: Role of the Synthesis Procedure on PEC CO2 Conversion. Materials 16, (2023).Zoli, M. et al. Facile and scalable synthesis of Cu2O-SnO2 catalyst for the photoelectrochemical CO2 conversion. Catal Today 413–415, 113985 (2023).Miró, R. et al. Solar-driven CO2 reduction catalysed by hybrid supramolecular photocathodes and enhanced by ionic liquids. Catal Sci Technol 13, 1708–1717 (2023).Sullivan, I. et al. Coupling electrochemical CO2 conversion with CO2 capture. Nat Catal 4, 952–958 (2021). Figure 1