Abstract
Post-synthetic modification of H3[(Cu4Cl)3(BTTri)8] or CuBTTri, where H3BTTri=1,3,5-tris(1H-1,2,3-triazol-5-yl)benzene, with piperazine (pip) has yielded the grafted framework H3[(Cu4Cl)3(BTTri)8(pip)12], pip-CuBTTri, which exhibits an improved CO2 uptake at pressures pertinent to postcombustion flue gas capture compared with the non-grafted material. In particular, the volumetric capacity of pip-CuBTTri was 2.5 times higher than that of CuBTTri at ca. 0.15bar and 293K. A chemisorption mechanism for CO2 adsorption was proposed on the basis of diffuse reflectance infrared spectra (DRIFTS) and the high initial isosteric heat of adsorption (−Qst, ≈96.5kJ/mol). Application of the Ideal Adsorbed Solution Theory (IAST) to a simulated mixture of 0.15bar CO2/0.75bar N2 revealed a selectivity factor of 130. Both pressure and temperature swing processes were found to be suitable for facile regeneration of the material over multiple adsorption–desorption cycles.
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