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 studyElectronic supplementary information (ESI) available: Details of the post-synthesis procedure, elemental and thermal analysis characterization, XRPD patterns, adsorption data, force fields and molecular simulations. See DOI: 10.1039/c5dt03137k

• 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: 1477-9226; 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 CO 2 adsorption properties under flue gas and air filtering conditions. On the basis of the [Mg 2 (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 CO 2 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 CO 2 adsorbents is derived through this computational and experimental investigation. A computational and experimental study is performed to determine the optimal composition that enhances the adsorption performance at low pressure.