Observation of reduced thermal conductivity in a metal-organic framework due to the presence of adsorbates

Hasan Babaei; Mallory E. DeCoster; Minyoung Jeong; Zeinab M. Hassan; Timur Islamoglu; Helmut Baumgart; Alan J.H. McGaughey; Engelbert Redel; Omar K. Farha; Patrick E. Hopkins; Jonathan A. Malen; Christopher E. Wilmer

doi:10.1038/s41467-020-17822-0

Observation of reduced thermal conductivity in a metal-organic framework due to the presence of adsorbates

Hasan Babaei, Mallory E. DeCoster, Minyoung Jeong, Zeinab M. Hassan, Timur Islamoglu, Helmut Baumgart, Alan J.H. McGaughey, Engelbert Redel, Omar K. Farha, Patrick E. Hopkins, Jonathan A. Malen, Christopher E. Wilmer^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

122 Scopus citations

Abstract

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.

Original language	English (US)
Article number	4010
Journal	Nature communications
Volume	11
Issue number	1
DOIs	https://doi.org/10.1038/s41467-020-17822-0
State	Published - Dec 1 2020

Funding

H.B. and C.E.W. gratefully acknowledge support from the National Science Foundation (NSF), awards CBET-1804011 and OAC-1931436, and also thank the Center for Research Computing (CRC) at the University of Pittsburgh for providing computational resources. J.A.M. gratefully acknowledges support from the Army Research Office, grant W911NF-17-1-0397. A.J.H.M. gratefully acknowledges support from the NSF, award DMR-1507325. O.K.F. gratefully acknowledges research support from the U.S. Department of Energy\u2019s Office of Energy Efficiency and Renewable Energy (EERE) under award no. DE\u2010EE0008816. P.E.H. appreciates support from the Army Research Office, Grant. No. W911NF-16-1-0320. Financial support by Deutsche Forschungsgemeinschaft (DFG) within the COORNET Priority Program (SPP 1928) is gratefully acknowledged by E.R. and He.B. (Helmut Baumgart). Z.M.H. acknowledges financial support from the Egyptian Mission Foundation. We would also like to thank Ran Cao for collecting additional PXRD data for this study.

ASJC Scopus subject areas

General Chemistry
General Biochemistry, Genetics and Molecular Biology
General Physics and Astronomy

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10.1038/s41467-020-17822-0

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Babaei, H., DeCoster, M. E., Jeong, M., Hassan, Z. M., Islamoglu, T., Baumgart, H., McGaughey, A. J. H., Redel, E., Farha, O. K., Hopkins, P. E., Malen, J. A., & Wilmer, C. E. (2020). Observation of reduced thermal conductivity in a metal-organic framework due to the presence of adsorbates. Nature communications, 11(1), Article 4010. https://doi.org/10.1038/s41467-020-17822-0

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abstract = "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.",

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Observation of reduced thermal conductivity in a metal-organic framework due to the presence of adsorbates

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