CO2 Uptake and Stability Enhancement in Vinyltrimethoxysilane‐Treated SBA‐15 Solid Amine‐Based Sorbents

Silica‐supported amine absorbents, including materials produced by tethering aminosilanes or infusion of poly(ethyleneimine), represent a promising class of materials for CO2 capture applications, including direct air and point source capture. Various silica surface treatments and functionalization strategies are explored to enhance stability and CO2 uptake in amine‐based solid sorbent systems. Here, the synthesis and characterization of novel vinyltrimethoxysilane‐treated Santa Barbara Amorphous‐15 (SBA‐15) supports and the corresponding enhancement in CO2 uptake compared to various SBA‐15‐based control supports are presented. The relationship between CO2 diffusion and amine efficiency in these systems is explored using a previously reported kinetic model. The synthesized materials are characterized with CO2 and H2O isotherms, diffuse reflectance infrared Fourier transform spectroscopy, 1H T1–T2 relaxation correlation NMR, and rapid thermal cycling experiments. The novel support materials are shown to enable high amine efficiencies, approaching a fourfold improvement over standard SBA‐15‐supported amines, while simultaneously exhibiting excellent stability when cycled rapidly under humid conditions. As the poly(ethyleneimine) loadings are held constant across the various samples, enhancements in CO2 uptake are attributed to differences in the way the poly(ethyleneimine) interacts with the support surface. A new surface treatment using vinyltrimethoxysilane on poly(ethyleneimine) (PEI)‐loaded B‐doped mesoporous silica is reported, which increases the activity of nitrogen sorption sites for CO2 capture under direct air capture and point‐source capture conditions. The novel surface treatment results in surface “patchiness” of PEI on the pore walls, giving rise to increased performance.