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

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 °C under 20 bar, with good methanol selectivity, negligible CO formation, and good stability for 12 h under harsh conditions.