Abstract
In this study, a previously reported Zr-MOF UiO-66(Zr)-(COOH)2 with optimal features for CO2 capture was ionized by neutralization with aqueous MOH solutions (M=Li+, Na+, K+). This post-synthetic modification route has endowed some of the resulting MOFs with higher CO2 uptake capacity. The CO2/N2 selectivity of UiO-66(Zr)-(COOK)2 calculated by Ideal Adsorption Solution Theory (IAST) demonstrates a significant enhancement of 83% compared with the pristine MOF. In addition, dynamic column breakthrough experiments were performed using a binary CO2/N2 mixed gas with a molar ratio of 15:85 to mimic the flue gas composition. The CO2/N2 selectivity of UiO-66(Zr)-(COONa)2 calculated based on breakthrough data is 99.6, which is among the highest CO2/N2 selectivities obtained experimentally using binary mixed gas breakthrough/co-adsorption experiments. Our results strongly confirm that ionization is an effective way of introducing strong CO2 adsorption sites into MOFs for higher CO2-MOF interactions and better CO2 separation performance.
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