Insight into Fluorocarbon Adsorption in Metal-Organic Frameworks via Experiments and Molecular Simulations

Barpaga, Dushyant; Nguyen, Van T.; Medasani, Bharat K.; Chatterjee, Sayandev; McGrail, B. Peter; Motkuri, Radha Kishan; Dang, Liem X.

doi:10.1038/s41598-019-46269-7

Title: Insight into Fluorocarbon Adsorption in Metal-Organic Frameworks via Experiments and Molecular Simulations

Journal Article · Tue Jul 16 00:00:00 EDT 2019 · Scientific Reports

DOI:https://doi.org/10.1038/s41598-019-46269-7· OSTI ID:1619544

Barpaga, Dushyant; Nguyen, Van T.;

; Chatterjee, Sayandev; McGrail, B. Peter;

; Dang, Liem X.

Abstract The improvement in adsorption/desorption of hydrofluorocarbons has implications for many heat transformation applications such as cooling, refrigeration, heat pumps, power generation, etc. The lack of chlorine in hydrofluorocarbons minimizes the lasting environmental damage to the ozone, with R134a (1,1,1,2-tetrafluoroethane) being used as the primary industrial alternative to commonly used Freon-12. The efficacy of novel adsorbents used in conjunction with R134a requires a deeper understanding of the host-guest chemical interaction. Metal-organic frameworks (MOFs) represent a newer class of adsorbent materials with significant industrial potential given their high surface area, porosity, stability, and tunability. In this work, we studied two benchmark MOFs, a microporous Ni-MOF-74 and mesoporous Cr-MIL-101. We employed a combined experimental and simulation approach to study the adsorption of R134a to better understand host-guest interactions using equilibrium isotherms, enthalpy of adsorption, Henry’s coefficients, and radial distribution functions. The overall uptake was shown to be exceptionally high for Cr-MIL-101, >140 wt% near saturation while >50 wt% at very low partial pressures. For both MOFs, simulation data suggest that metal sites provide preferable adsorption sites for fluorocarbon based on favorable C-F ··· M ⁺ interactions between negatively charged fluorine atoms of R134a and positively charged metal atoms of the MOF framework.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1619544

Alternate ID(s):: OSTI ID: 1557678

Report Number(s):: PNNL-SA-140049; 10289; PII: 46269

Journal Information:: Scientific Reports, Journal Name: Scientific Reports Vol. 9 Journal Issue: 1; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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Cited by: 28 works

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