Thermodynamics of methane adsorption on copper HKUST-1 at low pressure
- Univ. of California, Davis, CA (United States)
- Univ. of California, Davis, CA (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- East China Univ. of Science and Technology, Shanghai (China)
Metal–organic frameworks (MOFs) can be engineered as natural gas storage materials by tuning the pore structures and surface properties. Here we report the direct measurement of CH₄ adsorption enthalpy on a paddlewheel MOF (Cu HKUST-1) using gas adsorption calorimetry at 25 °C at low pressures (below 1 bar). In this pressure region, the CH₄–CH₄ intermolecular interactions are minimized and the energetics solely reflects the CH₄–MOF interactions. Our results suggest moderately exothermic physisorption with an enthalpy of -21.1 ± 1.1 kJ/mol CH₄ independent of coverage. The calorimetric investigation complements previous computational and crystallographic studies by providing zero coverage enthalpies of CH₄ adsorption. The analysis of the new and literature data suggests that in initial stages of adsorption the CH₄–HKUST-1 interaction tends to be more sensitive to the pore dimension than to the guest polarizability, suggesting a less specific chemical binding role for the open Cu site.
- Research Organization:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- Grant/Contract Number:
- 201308310077; 21201063; 20110074120020; FG02-05ER15667; AC52-06NA25396
- OSTI ID:
- 1221609
- Report Number(s):
- LA-UR-15-24040
- Journal Information:
- Journal of Physical Chemistry Letters, Vol. 6, Issue 13; ISSN 1948-7185
- Publisher:
- American Chemical SocietyCopyright Statement
- Country of Publication:
- United States
- Language:
- English
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