Mechanisms Governing Noble Gas Adsorption in a Copper-Based Metal-Organic Framework
Keerthana Krishnan1, Matthew J Hurlock1, Sun Hae Ra Shin1
1Pacific Northwest National Laboratory, 902 Battelle Blvd., Richland, Washington 99354, United States.
Metal-organic frameworks (MOFs) show promise for noble gas separation. High-dose gamma irradiation impacts MOF porosity, causing defects that alter gas adsorption properties, revealing sensitivity to ionizing radiation.
Area of Science:
- Materials Science
- Nuclear Engineering
- Radiochemistry
Background:
- Metal-organic frameworks (MOFs) are investigated as sorbents for noble gas separation in nuclear applications.
- Understanding MOF degradation under ionizing radiation is crucial for their safe deployment.
Purpose of the Study:
- To investigate the impact of high-dose gamma irradiation on the CuBTC MOF.
- To elucidate the degradation mechanisms and porosity changes in MOFs under ionizing radiation.
Main Methods:
- Exposure of CuBTC to 60Co gamma irradiation at doses from 1 to 5 MGy.
- Characterization using N2 gas adsorption, Xe and Kr uptake measurements, X-ray diffraction, and Fourier transform infrared spectroscopy.
Main Results:
- Irradiation decreased N2 and Xe gas uptake, with adsorption loss for Xe proportional to dose.
- Kr uptake increased up to 5 MGy, indicating pore constriction.
- Coordination defects were observed, correlating with pore blockage and altered surface area.
Conclusions:
- The bulk framework of CuBTC remains stable up to 5 MGy.
- MOF pore properties are highly sensitive to high-dose ionizing radiation.
- A methodology was established to understand MOF porosity changes under irradiation.
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