Journal
NATURE COMMUNICATIONS
Volume 11, Issue 1, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-020-17822-0
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Funding
- National Science Foundation (NSF) [CBET-1804011, OAC-1931436]
- Army Research Office [W911NF-16-1-0320, W911NF-17-1-0397]
- NSF [DMR-1507325]
- U.S. Department of Energy's Office of Energy Efficiency and Renewable Energy (EERE) [DE-EE0008816]
- Deutsche Forschungsgemeinschaft (DFG) within the COORNET Priority Program [SPP 1928]
- Egyptian Mission Foundation
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Whether the presence of adsorbates increases or decreases thermal conductivity in metal-organic frameworks (MOFs) has been an open question. Here we report observations of thermal transport in the metal-organic framework HKUST-1 in the presence of various liquid adsorbates: water, methanol, and ethanol. Experimental thermoreflectance measurements were performed on single crystals and thin films, and theoretical predictions were made using molecular dynamics simulations. We find that the thermal conductivity of HKUST-1 decreases by 40 - 80% depending on the adsorbate, a result that cannot be explained by effective medium approximations. Our findings demonstrate that adsorbates introduce additional phonon scattering in HKUST-1, which particularly shortens the lifetimes of low-frequency phonon modes. As a result, the system thermal conductivity is lowered to a greater extent than the increase expected by the creation of additional heat transfer channels. Finally, we show that thermal diffusivity is even more greatly reduced than thermal conductivity by adsorption. Metal-organic frameworks are attractive adsorbents for gas storage and separations, but appropriate heat dissipation is important for practical application. Here the authors use experiment and theory to show the impact of liquid adsorbates on thermal transport in metal-organic frameworks.
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