Tuning the target composition of amine-grafted CPO-27-Mg for capture of CO2 under post-combustion and air filtering conditions: a combined experimental and computational study

• Published in: Dalton transactions : an international journal of inorganic chemistry 2015-11, Vol.44 (43), p.18970-18982
• Main Authors: Bernini, M C, García Blanco, A A, Villarroel-Rocha, J, Fairen-Jimenez, D, Sapag, K, Ramirez-Pastor, A J, Narda, G E
• Format: Article
• Language: English
• ISSN: 1477-9234
• DOI: 10.1039/c5dt03137k

A computational and experimental screening of hypothetical and real compounds exhibiting different degrees of ethylenediamine grafted to the CPO-27-Mg or Mg-DOBDC skeleton is performed in order to determine the target composition that optimizes the CO2 adsorption properties under flue gas and air filtering conditions. On the basis of the [Mg2(dobdc)] formula, eighteen hypothetical models involving 15-100% of functionalization of the coordinatively unsaturated sites (CUS) were considered by means of Grand Canonical Monte Carlo simulations to evaluate the CO2 adsorption at 298 K. In addition, post-synthesis modification was applied to CPO-27-Mg leading to three kinds of samples exhibiting 15, 50, and 60% of CUS functionalization with ethylenediamine, named CPO-27-Mg-a, CPO-27-Mg-b and CPO-27-Mg-c. Compounds were characterized using elemental analysis, TGA, FTIR spectroscopy, PXRD and DSC. Finally, bare and functionalized CPO-27-Mg materials were evaluated using gas adsorption and microcalorimetry in the 0.001-1 bar range, which is pertinent for the mentioned applications. Valuable information related to design criteria for synthesis of tuned CO2 adsorbents is derived through this computational and experimental investigation.