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Investigation of Interfacial Chemistry with In Situ Infrared Spectroscopy

Jin, Hailiang
http://rave.ohiolink.edu/etdc/view?acc_num=akron1562531223401125

Abstract Details

2019, Doctor of Philosophy, University of Akron, Polymer Science.
The reaction happened on the interface of two phases plays an important role in the development of hydrogenous catalyst, electrochemistry, etc. Fourier Transform Infrared spectroscopy (FTIR) is one of the most powerful tools for the investigation of the interaction happened on the interface. In situ FTIR technology could monitor the breaking and formation of chemical bonding happened on the interface with the reaction happening simultaneously. The reaction intermediate and pathway could be carefully analyzed based on the in situ IR results. The existing of SO2 in the flue gas is a key factor causing the degradation of amine-based CO2 sorbent, which capture CO2 in flue gas at 40-60°C and release the adsorbed CO2 at 100-130 °C in a temperature swing separation process (i.e., temperature programed desorption). The interaction between SO2 and liquid amine film on the gas/liquid interface was studied with in situ FTIR for (1) the clarification of SO2 adsorption species, (2) the understanding of adsorption/desorption kinetics, (3) the effect of water on the adsorption of SO2. Sulfite and bisulfite are proposed as the species formed by SO2 adsorption, with bisulfite having low binding energy and sulfite having high binding energy with amine groups. The low binding energy of absorbed bisulfite which can be desorbed under 130°C shows that amine film possesses the site for the reversibly adsorption of SO2, i.e., desorption of adsorbed bisulfite. To achieve the complete desorption of SO2 from amine site, methylation process was applied on PEI to convert the primary and secondary amine groups to the tertiary amine. SO2 was observed to adsorb on the prepared methylated PEI reversibly. According to the obtained IR results, the adsorption of SO2 on tertiary amine formed sulfite/bisulfite cation and tertiary ammonium ions. A good SO2-resistance is manifested by the ability of tertiary amine site to desorb the adsorbed SO2 at the operation temperature of thermal swing CO2 capture process. Water is the most abundant liquid on the earth and the prerequisite for life on the planet. A material can be classified as either hydrophobic or hydrophilic, based on the favored or unfavored interaction between water and substrates. However, the understanding of the hydrophobic and hydrophilic phenomenon under a molecular level remained ambiguous. Contact angle measurements provide macroscopic information of hydrophobicity/hydrophilicity, in situ IR results and DFT simulations provide microscopic details of the system. By compositing the epoxy resin, carbon material and SiO2 based solid amine sorbent together, the polymer-carbon composite was developed with reasonable mechanical strength, the ability of capturing CO2 with a high capture capacity, and the fast heating/cooling ability to accelerate the overall CO2 capture process. The adding of carbon material provides the ability of generating heat with the direct applying of electricity to the composite, and increased the thermal conductivity for fast heating cooling. A modular cell design was achieved with a pouch cell setup, which could be used in a small area, or easily scaled up for industrial use.
Steven Chuang, PhD (Advisor)
Darrell Reneker, PhD (Committee Member)
Toshikazu Miyoshi, PhD (Committee Member)
Yu Zhu, PhD (Committee Chair)
Chrys Wesdemiotis, PhD (Committee Member)
254 p.
Polymer Chemistry; Polymers

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Citations

  • Jin, H. (2019). Investigation of Interfacial Chemistry with In Situ Infrared Spectroscopy [Doctoral dissertation, University of Akron]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=akron1562531223401125

    APA Style (7th edition)

  • Jin, Hailiang. Investigation of Interfacial Chemistry with In Situ Infrared Spectroscopy. 2019. University of Akron, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=akron1562531223401125.

    MLA Style (8th edition)

  • Jin, Hailiang. "Investigation of Interfacial Chemistry with In Situ Infrared Spectroscopy." Doctoral dissertation, University of Akron, 2019. http://rave.ohiolink.edu/etdc/view?acc_num=akron1562531223401125

    Chicago Manual of Style (17th edition)

akron1562531223401125
© 2019, all rights reserved.
This open access ETD is published by University of Akron and OhioLINK.