Autor: |
Das AK; Center for Molecular Electrocatalysis, Physical Sciences Division, Pacific Northwest National Laboratory (PNNL), Richland, Washington 99352, USA., Vemuri RS; Energy and Environment Directorate, Pacific Northwest National Laboratory (PNNL), Richland, WA 99352, USA., Kutnyakov I; Center for Molecular Electrocatalysis, Physical Sciences Division, Pacific Northwest National Laboratory (PNNL), Richland, Washington 99352, USA., McGrail BP; Energy and Environment Directorate, Pacific Northwest National Laboratory (PNNL), Richland, WA 99352, USA., Motkuri RK; Energy and Environment Directorate, Pacific Northwest National Laboratory (PNNL), Richland, WA 99352, USA. |
Abstrakt: |
Vapor-assisted dry-gel synthesis of the metal-organic framework-74 (MOF-74) structure, specifically Ni-MOF-74 produced from synthetic precursors using an organic-water hybrid solvent system, showed a very high yield (>90% with respect to 2,5-dihydroxyterepthalic acid) and enhanced performance. The Ni-MOF-74 obtained showed improved sorption characteristics towards CO2 and the refrigerant fluorocarbon dichlorodifluoromethane. Unlike conventional synthesis, which takes 72 hours using the tetrahydrofuran-water system, this kinetic study showed that Ni-MOF-74 forms within 12 hours under dry-gel conditions with similar performance characteristics, and exhibits its best performance characteristics even after 24 hours of heating. In the dry-gel conversion method, the physical separation of the solvent and precursor mixture allows for recycling of the solvent. We demonstrated efficient solvent recycling (up to three times) that resulted in significant cost benefits. The scaled-up manufacturing cost of Ni-MOF-74 synthesized via our dry-gel method is 45% of conventional synthesis cost. Thus, for bulk production of the MOFs, the proposed vapor-assisted, dry-gel method is efficient, simple, and inexpensive when compared to the conventional synthesis method. |