Charge polarization-modulated Pd-Ni(OH)2 hybrids in mesoporous silica SBA-15 for efficient low-temperature CO2 hydrogenation to formate

Converting CO2 to formic acid/formate is a considerably significant pathway for future energy storage and utilization; however, it is critical to tailor high-performance catalysts for realizing the process. Herein, highly dispersed Pd-Ni(OH)2 hybrids were immobilized in ordered mesoporous silica SBA-15 via a facile impregnation method. The prepared SBA-15-supported Pd-Ni(OH)(2) catalyst exhibited extraordinarily high catalytic perfor-mance and stability during the hydrogenation of CO2 toward formate. Significantly, Pd5Ni5/SBA-15, an opti-mized Pd5Ni5/SBA-15 catalyst afforded a superior formate generation rate of 150.5 mol(formate) mol(total)Pd(-1) h(- 1) at a low temperature (40 degrees C), which was about 3-fold higher than that of monometallic Pd counterpart. Such a catalytic activity outperforms most of the previously reported catalysts because of its charge polarization action and synergy between bimetallic components as well as ultrasmall and well-dispersed metal species with increased accessible active sites. The relevant experimental observations were well supported by density func-tional theory (DFT) calculations. In addition, the catalytic activity of SBA-15-supported metal catalysts remained unchanged even after the 5th cycle, demonstrating excellent cycling durability due to the confinement effect of mesoporous silica. The facile synthesis strategy and excellent catalytic performance hold great potential appli-cations of the prepared catalysts in CO2 hydrogenation to formate.

Automated summary

Converting CO2 to formic acid/formate is crucial for future energy storage, and developing high-performance catalysts is essential for this process. In this study, highly dispersed Pd-Ni(OH)2 hybrids were immobilized on ordered mesoporous silica SBA-15, showing exceptional catalytic performance and stability. The optimized Pd5Ni5/SBA-15 catalyst achieved a significantly higher formate generation rate compared to monometallic Pd counterpart, due to its charge polarization action and synergy between bimetallic components. The catalyst also exhibited excellent cycling durability. The results suggest great potential of these catalysts for CO2 hydrogenation to formate.