Carbon-Phosphorus-Nitrogen Materials as Highly Thermally Stable Catalyst Supports for CO2 Hydrogenation to Methanol

[EN] The direct conversion of CO2 into methanol through hydrogenation reactions by heterogeneous catalysts is considered a promising green approach for fuel production. The most researched catalyst for methanol formation is Cu, usually in combination with other metals dispersed on different substrates. However, several challenges, such as the low stability, activity, and selectivity of the catalyst, hinder further progress. Here, we present catalysts consisting of Cu and Fe nanoparticles deposited on lightweight carbon-phosphorous-nitrogen (CPN) materials as the support for CO2 hydrogenation to methanol. Detailed analysis reveals a correlation between the elemental composition of the CPN supports and their CO2 adsorption capability, which benefits CO2 conversion to methanol. The unique elemental composition ensures uniform dispersion of both Cu and Fe nanoparticles on CPN and prevents the oxidation of the Cu active sites during the reaction. The best performing sample of the catalysts exhibits a remarkable methanol production yield of 9.82 mol kgcat-1 h-1 at 250 degrees C under 20 bar, with good methanol selectivity, negligible CO formation, and good stability for 12 h under harsh conditions. This project has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 Research and Innovation Programme (grant agreement no. [849068]). The research was partly funded by the following: the Planning & Budgeting Committee/Israel Council for Higher Education (CHE) and Fuel Choice Initiative (Prime Minister Office of Israel), within the framework of "Israel National Research Center for Electrochemical Propulsion" (INREP); the Minerva Center no. 117873; the Israel Science Foundation grant no. 601/21; and the Spanish Ministerio de Economi ' a y Competitividad (MAT2016-77608-C3-1-P and MAT2016-75883-C2-2-P); J.A. and H.G. also gratefully acknowledges financial support from the Spanish Ministry of Economy and Competitiveness (Severo Ochoa SEV2016-0683 and RTI2018-89023-CO2-R1) and by the Generalitat Valenciana (Prometeo 2017-083). Azoulay, A.; García-Baldoví, A.; Albero-Sancho, J.; Azaria, N.; Tzadikov, J.; Tashakory, A.; Karjule, N... (2023). Carbon-Phosphorus-Nitrogen Materials as Highly Thermally Stable Catalyst Supports for CO2 Hydrogenation to Methanol. ACS Applied Energy Materials. 6(1):439-446. https://doi.org/10.1021/acsaem.2c03410