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CO2 Capture on Polymer-Silica Composites from Molecular Modeling to Pilot Scale

Willett, Erik Amos
http://orcid.org/0000-0002-4158-1302
http://rave.ohiolink.edu/etdc/view?acc_num=akron152147716339683

Abstract Details

2018, Doctor of Philosophy, University of Akron, Polymer Science.
Fossil energy from coal, gas, and oil-based fuel stocks remains a vital cornerstone of the global energy infrastructure while contributing over half of annual CO2 emissions. Rising global CO2 concentrations and aberrant trends in climate have sparked recent scrutiny of the energy industry sustainability. Carbon capture, utilization, and storage (CCUS) at the site of power plants has been proposed as a strategy for mitigating atmospheric CO2. This dissertation covers simulated and experimental models designed to address key problems in both the fundamental science and applied engineering of amine-functionalized silica sorbents for carbon capture from few molecule DFT (density functional theory) calculation to kilogram-scale technology validation. DFT was used to emulate small molecule and polymeric amines with good agreement in four successive series of models. (i) The concept of CO2 adsorption strength on secondary amines was investigated which revealed lone amine sites produce weakly adsorbed species while dense amine pairs yield strongly adsorbed species. (ii) Mixed amine types are common in blended or polymeric amine systems and convolute data interpretation. The hydrogen bonding ability of ammonium carbamate pairs demonstrated significant dependence on amine type and local hydrogen bond partners. (iii) Fixation of amines onto substrates is a ubiquitous strategy for preparing CO2 sorbents. The effect of geometric constraint imposed by immobilization was investigated for simulated propylamine pairs. Binding energy was linearly dependent on the alignment of ammonium carbamate. FTIR features were categorized into four groups. (iv) Selective formation of carbamic acid was studied by modeling reactants, intermediates, transition states (TS), and products of the amine-CO2 reaction on simulated diamine substrates. It was shown that significant reduction in TS activation energy occurred by Grotthus-like proton hopping. Coal-fire power plant CO2 capture was experimentally modeled on the kW scale using kilogram-scale sorbent beds in a custom-built `pilot unit’ for technology validation in an industrial collaboration. The pilot unit demonstrated emergent challenges in scaling from sub-gram scale to kilograms.
Steven Chuang (Advisor)
Mesfin Tsige (Committee Chair)
Tianbo Liu (Committee Member)
Stephen Cheng (Committee Member)
David Perry (Committee Member)
254 p.
Chemical Engineering; Chemistry; Materials Science; Physical Chemistry; Polymers
Carbon capture; CCUS; amine; DFT simulation; FTIR spectroscopy; ammonium carbamate; material science; reversible CO2 capture; thermal swing adsorption; zwitterion; amine-CO2 reaction; solid-supported; silica; chemical engineering; reaction

Recommended Citations

Citations

  • Willett, E. A. (2018). CO2 Capture on Polymer-Silica Composites from Molecular Modeling to Pilot Scale [Doctoral dissertation, University of Akron]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=akron152147716339683

    APA Style (7th edition)

  • Willett, Erik. CO2 Capture on Polymer-Silica Composites from Molecular Modeling to Pilot Scale. 2018. University of Akron, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=akron152147716339683.

    MLA Style (8th edition)

  • Willett, Erik. "CO2 Capture on Polymer-Silica Composites from Molecular Modeling to Pilot Scale." Doctoral dissertation, University of Akron, 2018. http://rave.ohiolink.edu/etdc/view?acc_num=akron152147716339683

    Chicago Manual of Style (17th edition)

akron152147716339683
378
© 2018, all rights reserved.
This open access ETD is published by University of Akron and OhioLINK.