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In-Situ Infrared Studies of Adsorbed Species in CO2 Capture and Green Chemical Processes

Zhang, Long
http://orcid.org/0000-0003-2770-3593
http://rave.ohiolink.edu/etdc/view?acc_num=akron1481213980572202

Abstract Details

2016, Doctor of Philosophy, University of Akron, Polymer Science.
Clean energy and environment is a 21st-century contemporary challenge we human being faces. Tremendous effort has been paid to explore and develop technologies to produce green energy, to reduce the emissions of wastes, and to utilize these wastes and renewable sources. Catalysis technologies and CO2 capture and utilization technologies are among the most important stepping stones to achieve the challenging goals to secure the environment for human survival and development. The advancement in these technologies requires a molecular-level or quantum-level fundamental understanding of the processes involved. One critical aspect of importance is the nature of the adsorbed species and their evolution in these green chemical processes. Fourier transform infrared (FTIR) spectroscopy is a powerful and versatile tool that can provide the insights to address these scientific issues. This dissertation, with a focus on the applications of in-situ FTIR spectroscopy, discusses about a few important topics in CO2 capture and other green processes, including (i) the catalytic asymmetric hydrogenation of a-amino ester, a potential chemical building block and starting material for biocompatible polymers, (ii) the oxidative and CO2-induced degradation of supported polyethylenimine (PEI) adsorbents for CO2 capture, (iii) the utilization of CO2 by the catalytic conversion of CO2 to carbonates, a precursor for polycarbonates and polyurethanes, (iv) the catalytic conversion of 2,3-butanediol to 1,3-butadiene, the monomer for synthetic rubbers, and (v) the electron-induced IR absorbance in photocatalytic processes on TiO2. A wide array of FTIR techniques, including diffuse reflectance, attenuated total reflectance, and transmission IR has been applied. The FTIR results revealed the vital hydrogen bonding interactions in the catalytic asymmetric hydrogenation of a-amino ester which led to the prochiral structures. The oxidative degradation and CO2-induced degradation pathways were elucidated with the help of various FTIR studies conducted. The mechanism of the oxidative degradation of amines was proposed for the first time that the solid amines underwent the deactivation to imines and further oxidation to amides. The effects of amine loading, temperature, and water vapor on CO2-induced degradation were clarified. The FTIR spectra evidenced the successful conversion of CO2 to dimethyl carbonate and 2,3-butanediol to 1,3-butadiene, and helped the comprehension of the kinetics and the nature of the dehydrating agent in the reactions. In-situ FTIR was also used to differentiate the contributions from the conduction-band electrons and shallow-trapped electrons to the polaronic light absorbance. A modelling method was developed to analyze the IR spectra. The modelling results revealed the correlation of these differently sourced absorbance and the generation of photocurrent and the charge transportation process in photocatalysis.
Steven Chuang, Ph.D. (Advisor)
Toshikazu Miyoshi, Ph.D. (Committee Chair)
Xiong Gong, Ph.D. (Committee Member)
William Landis, Ph.D. (Committee Member)
Mesfin Tsige, Ph.D. (Committee Member)
198 p.
Chemical Engineering; Energy; Engineering; Environmental Science; Polymers
Infrared Spectroscopy; CO2 Capture; CO2 Utilization; Catalysis; Polyethylenimine; Hydrogenation; Photocatalysis

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Citations

  • Zhang, L. (2016). In-Situ Infrared Studies of Adsorbed Species in CO2 Capture and Green Chemical Processes [Doctoral dissertation, University of Akron]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=akron1481213980572202

    APA Style (7th edition)

  • Zhang, Long. In-Situ Infrared Studies of Adsorbed Species in CO2 Capture and Green Chemical Processes. 2016. University of Akron, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=akron1481213980572202.

    MLA Style (8th edition)

  • Zhang, Long. "In-Situ Infrared Studies of Adsorbed Species in CO2 Capture and Green Chemical Processes." Doctoral dissertation, University of Akron, 2016. http://rave.ohiolink.edu/etdc/view?acc_num=akron1481213980572202

    Chicago Manual of Style (17th edition)

akron1481213980572202
175
© 2016, all rights reserved.
This open access ETD is published by University of Akron and OhioLINK.