Copper benzene-1,3,5-tricarboxylate (HKUST-1) – Graphene oxide pellets for methane adsorption

Domán, Andrea and Madarász, János and Sáfrán, György and Wang, Ying and Nagyné László, Krisztina (2021) Copper benzene-1,3,5-tricarboxylate (HKUST-1) – Graphene oxide pellets for methane adsorption. MICROPOROUS and Mesoporous Materials. ISSN 1387-1811

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Abstract

Copper benzene-1,3,5-tricarboxylate (HKUST-1) is one of the materials holding the greatest potential for clean energy gases among microporous storage materials. Although this material is commercially available as a powder with particle size 10–20 μm, for easier handling adsorbents are preferentially employed as pellets or monoliths. Even under binder free conditions there could be a high price to pay for compacting: loss in crystallinity and in porosity. To determine the protection potential of graphene oxide (GO) a HKUST-1@GO composite was studied. The material of 16% GO was obtained in a single step solvothermal synthesis. The pristine HKUST-1 as well as HKUST 1@GO formed consistent, integrated pellets when compressed at 25 and 50 bar without any binder. Powder-XRD and N2 adsorption were used to monitor the changes in crystallinity and pore structure. It was found that GO has a protective effect against the 25 or 50 bar applied pressure, as 75% of the pore volume and the apparent surface area is saved in HKUST 1@GO (vs. 43% and 47%, respectively, in HKUST-1) after compression. Presumably, the flexible GO sheets with high mechanical stability act as compressible spacers between the crystals thus preventing their amorphisation. Comparison of the adsorption properties of the HKUST-1 and HKUST-1@GO powders and pellets revealed that the performed compression deteriorated the structure of the MOF and thus reduced the CH4 uptake. Further studies are needed to optimize the compression pressure for a more reasonable loss in the gas uptake capacity.

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