Discipline: Technology and Engineering
Subcategory: Materials Science
Jorge L. Rosa-Raices - University of Puerto Rico - Mayaguez Campus
Co-Author(s): Paul de J. Meza-Morales and María C. CuretArana, University of Puerto Rico - Mayagüez Campus, PR
Metal-organic frameworks (MOFs) have emerged as potential alternatives for the capture and storage of CO2 from flue gas emissions., An archetypal example is [M(bdc)(ted)0.5] (M = Ni or Zn; bdc = 1,4-benzenedicarboxylate; ted = triethylenediamine), for which experimental work has shown considerable CO2 uptake capacity, accompanied by structural transformations in the two isostructures. In this work, we provide a description of the adsorption dynamics of CO2 onto [M(bdc)(ted)0.5] based on grand-canonical Monte Carlo (GCMC) simulations. To account for electrostatic CO2-sorbent interactions, we obtain partial charges for the framework atoms by charge equilibration, and by fitting electrostatic potentials derived from density functional calculations. The efficacy of these methods to render the charge distribution of [M(bdc)(ted)0.5] is assessed on the basis of agreement with experimental isotherms. In light of a thermodynamic model previously used to quantitatively describe CO2-induced structural transformations in a similar MOF, we posit a structural rearrangement for [M(bdc)(ted)0.5]– CO2 and obtain isotherms with GCMC simulations that closely resemble experimental data.
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Funder Acknowledgement(s): This research was supported by NSF-CREST (Grant number HRD-1345156) and NASA EPSCoR (Grant number NNX13AD38A). This research used computational resources of the National Energy Research Scientific Computing Center, which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE -AC02-05CH11231, and the High-Performance Computing Facility of the Institute for Functional Nanomaterials, which is supported by NSF through grants EPS-1002410 and EPS 101009.
Faculty Advisor: María Curet-Arana, firstname.lastname@example.org