Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 124, Issue 1, Pages 398-403Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.9b08008
Keywords
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Funding
- Gene and Linda Voiland School of Chemical Engineering and Bioengineering at Washington State University
- Alexandra Navrotsky Institute for Experimental Thermodynamics
- Chambroad Scholarship
- National Natural Science Foundation of China [91634112, 21878097]
- Natural Science Foundation of Shanghai [16ZR1408100]
- Open Project of State Key Laboratory of Chemical Engineering [SKL-ChE16C01]
- Key Project of Education Department of Sichuan Province [15ZA0229]
- National Science Foundation [DMR0936384]
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mmen-Mg-2(dobpdc) (mmen = N,N'-dimethylethylenediamine, dobpdc = 4,4'-dioxidobiphenyl-3,3'-dicarboxylate) is a diamine-appended metal-organic framework (MOF) material with promising future as an efficient CO2 capture sorbent for industry applications. Here, using adsorption calorimetry, the energetic landscape of mmen-Mg-2(dobpdc) hydration has been revealed. Specifically, at near-zero water coverage, hydration results in the most exothermic differential enthalpy of adsorption of -110.9 +/- 3.1 kJ/mol water. A differential enthalpy plateau at -65.8 +/- 4.7 kJ/mol water is observed at the intermediate degree of hydration, which corresponds to water-diamine chemisorption through hydrogen bonding. Eventually, mmen-Mg-2(dobpdc) hydration is concluded at the second differential enthalpy plateau at -44.2 +/- 1.8 kJ/mol water suggesting condensation of water within the internal channel space of mmen-Mg-2(dobpdc). The position of the second plateau at about -44.0 kJ/mol water strongly suggests formation of liquid-like water clusters within the hydrophilic nanoconfinement environment. This comprehensive study energetically distinguishes the guest-host interfacial bonding and guest-guest intermolecular interactions for the water-mmen-Mg-2(dobpdc) system, which provides fundamental thermodynamic data to enhance our understanding of the behavior of CO2 capture sorbents in the presence of moisture.
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