Novel Amine-Functionalized Magnesium Oxide Adsorbents for CO2 Capture at Ambient Conditions

Abstract

• MgO was synthesized using three facile methods • MgO was functionalized with different amines (APTES, DETA and PEI) • APTES-MgO and DETA-MgO adsorbed more than 2 and 1.5 times CO 2 relative to bare MgO • APTES-MgO preserved its full adsorption capacity even after 6 regeneration cycles • Regeneration is carried out using N 2 under mild conditions (30 min, 120 °C, 1 atm) In this study, we synthesized novel magnesium oxide-based adsorbents and utilized them for CO 2 capture at ambient conditions (1 atm, 30 °C). Magnesium oxide (MgO) was synthesized using a facile sol-gel technique starting from magnesium nitrate and ammonium hydroxide, sodium hydroxide or oxalic acid. MgO adsorbent synthesized in the presence of ammonium hydroxide (labeled as MgO-A) showed the highest surface area (350 m 2 /g), which has been correlated with the highest CO 2 adsorption capacity (30 mg/g) relative to those synthesized in the presence of sodium hydroxide (MgO-N) or oxalic acid (MgO-O). The characterization of the MgO samples (MgO-A, MgO-N and MgO-O) using XRD, FTIR, SEM, BET, and elemental analysis revealed that the synthesis route has a significant impact not only on surface area but also on the crystallinity, morphology, and textural properties (surface area, porosity and pore size distribution) of these MgO adsorbents. Nonetheless, the key novelty of the work reported herein is the functionalization of MgO with 3-aminopropyl-triethoxysilane (APTES), diethylenetriamine (DETA) and polyethylenimine (PEI) and their utilization for CO 2 capture at ambient conditions. The functionalization of MgO-A with the three amines significantly altered its characteristics (i.e., crystallinity, morphology, and textural properties). More importantly, the functionalization of MgO-A with APTES and DETA resulted in an increase in CO 2 adsorption from 30 (in the case of the unmodified MgO-A) to 65 and 47.6 mg/g, respectively. These values correspond, respectively, to 0.81 and 1.13 mol CO 2 captured/mol amine loaded on MgO-A. However, the functionalization of MgO-A with the polymeric amine (PEI) caused a significant reduction in the adsorbent surface area, leading to a decrease in CO 2 adsorption. Regeneration studies (using APTES-MgO-A as an example) demonstrated that contacting the spent adsorbent with N 2 gas at 120 °C for a short time can fully restore its original adsorption capacity, suggesting the potential commercial use of APTES-MgO-A for CO 2 capture with a minimal energy requirement.