Structure Property-CO2 Capture Performance Relations of Amine-Functionalized Porous Silica Composite Adsorbents.

In order to investigate the influence of support structure properties on CO2 capture performances of solid amine adsorbents, a novel three-dimensional disordered porous silica (3dd) with hierarchical pore networks was developed and then compared to other three materials as adsorbent support, namely, hierarchical porous silica (HPS), MCM-41, and SBA-15. They were all functionalized with tetraethylenepentaamine (TEPA) to prepare CO2 adsorbents. The adsorbents' ability to capture CO2 was examined on a fixed-bed reactor. When these supports had 60 wt% TEPA loading, the amounts of CO2 captured followed the order 3dd > HPS > SBA-15 > MCM-41 at 75 °C; the adsorption capacities were 5.09, 4.9, 4.58, and 2.49 mmol/g, respectively. The results indicate that a larger pore volume can promote the dispersion of amine species to expose more active sites for CO2 capture. The larger pore size can decrease the CO2 diffusion resistance. High surface area is not an important factor in determining capture performance. In addition, compared with conventional single-size mesopores, the hierarchical pore networks can disperse the TEPA species in different levels of the channel to limit undesired loss/aggregation of impregnated TEPA species. Thus, the 3dd support exhibits the best stability and highest regeneration conversion compared to the other three supports. This work demonstrates that the rational design of adsorbent support systems can effectively relieve the trade-off between amine loading and diffusion resistance. One method to surmount this trade-off is to utilize an adsorbent platform with hierarchical pore networks. Thus, this work may provide a feasible strategy for the design of CO2 solid amine adsorbents with high capture amount and amine utilization efficiency.