期刊
CHEMPHYSCHEM
卷 13, 期 14, 页码 3275-3281出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cphc.201200243
关键词
adsorption; breathing; carbon dioxide; Coudert model; metal-organic frameworks
资金
- Laboratory Directed Research Development, Office of Basic Energy Sciences (BES)
- Office of Fossil Energy, U.S. Department of Energy (DOE)
- Department of Energy [DE-AC05-76RL01830]
The framework expansion and contraction upon carbon dioxide uptake was studied in a partially fluorinated metalorganic framework, FMOF-2. The results show framework expansion and contraction (breathing) as a function of pressure and temperature. Even at temperatures as low as -30?degrees C, two phase transitions seem to take place with a pressure step (corresponding to the second transition) that is greatly dependent on temperature. This behavior is described by the model proposed by Coudert and co-workers showing that the material seems to undergo two phase transitions that are temperature-dependent. The isosteric heats of adsorption at high pressures show a minimum that is concurrent with the region of CO2 loadings where the second pressure step occurs. It was deduced that these lower enthalpy values are a consequence of the energy cost related to the expansion or reopening of the framework. Lastly, the large and reversible breathing behavior may be a product of the combination of the high elasticity of zinc (II) coordination and the apparent high flexibility of the V-shaped organic building block.
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