<i>In-Situ</i> Infrared Studies of Adsorbed Species in CO<sub>2</sub> Capture and Green Chemical Processes
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University of Akron / OhioLINK
2016
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| Online Access: | http://rave.ohiolink.edu/etdc/view?acc_num=akron1481213980572202 |
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ndltd-OhioLink-oai-etd.ohiolink.edu-akron14812139805722022021-08-03T06:39:10Z <i>In-Situ</i> Infrared Studies of Adsorbed Species in CO<sub>2</sub> Capture and Green Chemical Processes Zhang, Long Polymers Chemical Engineering Engineering Energy Environmental Science Infrared Spectroscopy CO2 Capture CO2 Utilization Catalysis Polyethylenimine Hydrogenation Photocatalysis Clean energy and environment is a 21<sup>st</sup>-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 CO<sub>2</sub> 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 <i>in-situ</i> FTIR spectroscopy, discusses about a few important topics in CO<sub>2</sub> 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 CO<sub>2</sub>-induced degradation of supported polyethylenimine (PEI) adsorbents for CO<sub>2</sub> capture, (iii) the utilization of CO<sub>2</sub> by the catalytic conversion of CO<sub>2</sub> 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 TiO<sub>2</sub>. 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 CO<sub>2</sub>-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 CO<sub>2</sub>-induced degradation were clarified. The FTIR spectra evidenced the successful conversion of CO<sub>2</sub> 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. <i>In-situ</i> 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. 2016 English text University of Akron / OhioLINK http://rave.ohiolink.edu/etdc/view?acc_num=akron1481213980572202 http://rave.ohiolink.edu/etdc/view?acc_num=akron1481213980572202 unrestricted This thesis or dissertation is protected by copyright: all rights reserved. It may not be copied or redistributed beyond the terms of applicable copyright laws. |
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NDLTD |
| language |
English |
| sources |
NDLTD |
| topic |
Polymers Chemical Engineering Engineering Energy Environmental Science Infrared Spectroscopy CO2 Capture CO2 Utilization Catalysis Polyethylenimine Hydrogenation Photocatalysis |
| spellingShingle |
Polymers Chemical Engineering Engineering Energy Environmental Science Infrared Spectroscopy CO2 Capture CO2 Utilization Catalysis Polyethylenimine Hydrogenation Photocatalysis Zhang, Long <i>In-Situ</i> Infrared Studies of Adsorbed Species in CO<sub>2</sub> Capture and Green Chemical Processes |
| author |
Zhang, Long |
| author_facet |
Zhang, Long |
| author_sort |
Zhang, Long |
| title |
<i>In-Situ</i> Infrared Studies of Adsorbed Species in CO<sub>2</sub> Capture and Green Chemical Processes |
| title_short |
<i>In-Situ</i> Infrared Studies of Adsorbed Species in CO<sub>2</sub> Capture and Green Chemical Processes |
| title_full |
<i>In-Situ</i> Infrared Studies of Adsorbed Species in CO<sub>2</sub> Capture and Green Chemical Processes |
| title_fullStr |
<i>In-Situ</i> Infrared Studies of Adsorbed Species in CO<sub>2</sub> Capture and Green Chemical Processes |
| title_full_unstemmed |
<i>In-Situ</i> Infrared Studies of Adsorbed Species in CO<sub>2</sub> Capture and Green Chemical Processes |
| title_sort |
<i>in-situ</i> infrared studies of adsorbed species in co<sub>2</sub> capture and green chemical processes |
| publisher |
University of Akron / OhioLINK |
| publishDate |
2016 |
| url |
http://rave.ohiolink.edu/etdc/view?acc_num=akron1481213980572202 |
| work_keys_str_mv |
AT zhanglong iinsituiinfraredstudiesofadsorbedspeciesincosub2subcaptureandgreenchemicalprocesses |
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1719440867913105408 |