Title:
ETHYLENE/ETHANE SEPARATION IN METAL-ORGANIC FRAMEWORK BY COMPUTATIONAL MODELING
ETHYLENE/ETHANE SEPARATION IN METAL-ORGANIC FRAMEWORK BY COMPUTATIONAL MODELING
Author(s)
You, Wenqin
Advisor(s)
Sholl, David S.
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Abstract
Metal-organic frameworks (MOFs) with open metal sites (OMS) are known to
have selectivity in olefin/paraffin separations because of π-π interactions between olefin
double bonds and OMS. This dissertation utilized computational methods to accomplish
three goals: (1) screening MOF materials with open metal sites for ethylene/ethane
separation; (2) test the adsorption performance of promising MOF materials with OMS
for the multicomponent separation; and (3) estimate their process performance.
We first used Density Functional Theory (DFT) to assess the binding energy of
ethylene, water, and carbon monoxide on a set of more than 60 MOFs with open Cu sites
in the form of Cu dimers. The main observation is that MOF topology and linker species
are secondary factors in determining the binding energy. We further used metal substitution
and linker functionalization to tune the relative binding affinities in MOFs with OMS,
which is turned to be more effective. Mixed-metal strategy is proved to be promising to
tune the binding affinity of guest molecule in bimetallic systems. The process performance
of the materials was also estimated with idealized and full pressure swing adsorption
models. Additionally, materials based on kinetic ethylene/ethane separation were also
investigated in this dissertation. This work paves the way for more robust material design
for ethylene/ethane separation.
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Date Issued
2020-03-26
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Resource Subtype
Dissertation