Highly dispersed Pd catalysts on zirconia for sustainable CO2 hydrogenation
摘要
The hydrogenation of CO2 into methanol presents a promising route for mitigating greenhouse gas emissions and advancing sustainable fuel production. However, catalyst deactivation due to water formation remains a significant challenge. Zirconia, with its limited hydrophilicity, serves as an effective support for CO2 hydrogenation. Highly dispersed transition metals, particularly palladium, have been identified as optimal binding sites for carbon dioxide molecules and hydrogen atoms, enhancing their interactions and eventual conversion to methanol. These offer advantages over traditional heterogeneous catalysts that incorporate costly precious metals with low metal atom consumption efficiency. This study examines the hydrogenation of CO2 to methanol utilising newly synthesised highly dispersed Pd catalysts doped on ZrO2 nanoparticles and zirconia solid solutions (InZrOx, ZnZrOx, and CdZrOx). The catalysts were synthesised and characterised using high-resolution transmission electron microscopy and energy-dispersive X-ray spectroscopy, revealing excellent Pd dispersion. Their catalytic performance was evaluated under optimised conditions. Pd/ZrO2 exhibited a methanol yield of 0.132 gMeOH·gcat−1·h−1. By modifying the support, Pd/CdZrOx achieved a significantly higher yield of 0.409 gMeOH·gcat−1·h−1, demonstrating enhanced catalytic efficiency. This improvement is attributed to the superior reducibility of CdZrOx, with a reduction temperature of 252 °C compared to 540 °C for ZrO2. Here, we show that optimising zirconia supports enhances CO2 hydrogenation activity, offering a scalable approach for efficient methanol synthesis. This work underscores the potential of Pd-doped zirconia catalysts for sustainable CO2 conversion, contributing to carbon–neutral fuel technologies.