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CO2 (H2S)-SELECTIVE MEMBRANES FOR FUEL CELL HYDROGEN PURIFICATION AND FLUE GAS CARBON CAPTURE: AN EXPERIMENTAL AND PROCESS MODELING STUDY

Ramasubramanian, Kartik
http://rave.ohiolink.edu/etdc/view?acc_num=osu1374193903

Abstract Details

2013, Doctor of Philosophy, Ohio State University, Chemical and Biomolecular Engineering.
CO2 capture from fuel and flue gases is critical to reducing the anthropogenic influence on climate change. Solvent absorption-, adsorption- and membrane-based processes have been widely studied for this application. Compared to the former two alternatives which are equilibrium-based, membrane separation is rate-based and does not involve phase change. Membranes hold great promise for CO2 capture due to their potentially lower energy consumption compared to other processes, operational simplicity with no handling of steam and condensed phases, lower water consumption, compactness, and ease of maintenance due to absence of moving parts. CO2 (H2S)-selective membranes with appropriate separation capabilities can be used to separate CO2 from waste gases in a fossil fuel-based power plant or both CO2 and H2S from syngas streams containing hydrogen. They can also be integrated with water gas shift (WGS) reaction for effective CO, CO2 and H2S clean up. In the context of hydrogen purification for fuel cells, a detailed 2-D model incorporating mass, energy and pressure drop equations for describing the transport in an intricate spiral-wound WGS membrane reactor was developed and validated using prior experimental data. Such a configuration is also used in state-of-the-art water purification processes and was the preferred choice for the advanced gas separation membranes studied in this work. A simplified 1-D version of the same model was then combined with a detailed cost methodology to study the feasibility of membrane processes for post-combustion CO2 capture (PCC) in a coal-based power plant. From this study, valuable insights into the membrane properties required to meet the economic goals of PCC were gained. As a part of the experimental work, we first scaled up an existing amine-based facilitated transport membrane to purify hydrogen for fuel cells. The membranes were then characterized for their separation performance using a gas permeation set-up and compared with lab-scale membranes. Later, we focused on developing membranes for PCC. It is known that inorganic membranes can offer advantageous separation/substrate capabilities while lacking the ease of scale-up and economic viability of polymer membranes. Driven by the idea to combine the good qualities of the above two types of membranes, detailed protocols for depositing thin (<1 &#xb5;m) zeolite Y layers (~40 and ~200 nm particle sizes) on polymer supports were developed. The effects of support surface morphology (pore size and surface porosity), inorganic particle size and layer thickness on the quality of deposition were studied using imaging via optical as well as electron microscopy. Lastly, the above multilayer hybrid materials were used as substrates for amine-based selective layers. In order to improve the membrane for PCC, different amines were used and compared on the basis of their separation capabilities. Also, the membrane tolerance towards SO2, a common minor component in flue gas, was studied by continuous monitoring of separation performance in the presence of simulated gas mixtures with different SO2 levels.
W.S. Winston Ho, PhD (Advisor)
Stuart Cooper, PhD (Committee Member)
David Tomasko, PhD (Committee Member)
270 p.
Chemical Engineering
membranes; carbon capture; post-combustion; spiral-wound module; sweep gas; vacuum; dip-coating; zeolite; inorganic-polymer; CO2 capture; fuel cell hydrogen; amine; facilitated transport membrane; hybrid substrates; polydimethylsiloxane

Recommended Citations

Citations

  • Ramasubramanian, K. (2013). CO2 (H2S)-SELECTIVE MEMBRANES FOR FUEL CELL HYDROGEN PURIFICATION AND FLUE GAS CARBON CAPTURE: AN EXPERIMENTAL AND PROCESS MODELING STUDY [Doctoral dissertation, Ohio State University]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=osu1374193903

    APA Style (7th edition)

  • Ramasubramanian, Kartik. CO2 (H2S)-SELECTIVE MEMBRANES FOR FUEL CELL HYDROGEN PURIFICATION AND FLUE GAS CARBON CAPTURE: AN EXPERIMENTAL AND PROCESS MODELING STUDY . 2013. Ohio State University, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=osu1374193903.

    MLA Style (8th edition)

  • Ramasubramanian, Kartik. "CO2 (H2S)-SELECTIVE MEMBRANES FOR FUEL CELL HYDROGEN PURIFICATION AND FLUE GAS CARBON CAPTURE: AN EXPERIMENTAL AND PROCESS MODELING STUDY ." Doctoral dissertation, Ohio State University, 2013. http://rave.ohiolink.edu/etdc/view?acc_num=osu1374193903

    Chicago Manual of Style (17th edition)

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This open access ETD is published by The Ohio State University and OhioLINK.