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Facilitated Transport Membranes for Carbon Capture from Flue Gas and H2 Purification from Syngas: From Membrane Synthesis to Process Design

Han, Yang
http://orcid.org/0000-0002-6390-247X
http://rave.ohiolink.edu/etdc/view?acc_num=osu1543333780761185

Abstract Details

2018, Doctor of Philosophy, Ohio State University, Chemical Engineering.
Polymeric facilitated transport membranes (FTMs) driven by reversible amine-CO2 reactions were developed in this study for selective CO2 separation from flue gas (CO2/N2) and syngas (CO2/H2). For post-combustion carbon capture, a FTM was synthesized in a composite membrane configuration with a 170 nm selective layer coated on a nanoporous substrate. In the selective layer, polyvinylamine with amine-sites covalently bonded to the polymer backbone was used as fixed-site carrier and an amino acid salt, synthesized by deprotonating sarcosine with 2-(1-piperazinyl)ethylamine, was blended as mobile carrier. Multi-walled carbon nanotubes wrapped by a copolymer poly(vinylpyrrolidone-co-vinyl acetate) were dispersed in the selective layer as reinforcement fillers to refrain the selective layer penetration upon vacuum suction. The membrane demonstrated a CO2 permeance of 1451 GPU (1 GPU = 10-6 cm3(STP)·cm-2·s-1·cmHg-1) and a CO2/N2 selectivity >140 at testing conditions relevant to this separation modality. A field trial with 1.4 m2 spiral-wound membrane modules fabricated from this FTM was conducted with actual flue gas at National Carbon Capture Center in Wilsonville, AL. The separation performances of the modules agreed well with those of the lab-scale flat-sheet membranes. A 500-h stability was demonstrated in spite of the interference of system upset and flue gas outage. Two membrane processes were designed for the FTM to decarbonizing coal-derived flue gas with 90% CO2 recovery. Power plant combustion air and a CO2-depleted retentate within the membrane system were identified as effective sweep gases to provide the transmembrane driving force. Both membrane processes yielded a capture cost ca. 40/tonne CO2 in 2011 dollars, which nearly met the target set by the U.S. Department of Energy for 2025. For pre-combustion carbon capture, FTMs were tailored for a single-stage membrane process to decarbonize coal-derived syngas. In these membranes, water-swellable crosslinked polyvinylalcohol was used as polymer matrix, along with polyvinylamine as fixed-site carrier. The 2-(1-piperazinyl)ethylamine salts of sarcosine and 2-aminoisobutyric acid served as the mobile carriers, while 1-(2-hydroxyethyl)piperazine and poly(ethylene glycol) dimethyl ether were incorporated as enhancers for the sorption of CO2. Nanoporous graphene oxide was dispersed to avoid membrane compaction upon a high feed pressure. The synthesized membranes showed different extents of carrier saturation at a high feed CO2 partial pressure. To capitalize this feature, a single-stage membrane process with hybrid membrane allocation was designed. Initial techno-economic analysis showed that the membrane process could achieve 90% CO2 removal with >99.3% H2 recovery. A 15.7% increase in the cost of electricity was estimated, which was more cost-efficient than conventional physical solvents.
W.S. Winston Ho (Advisor)
Liang-Shih Fan (Committee Member)
Andre Palmer (Committee Member)
211 p.
Chemical Engineering; Polymers
Membrane; carbon capture; gas separation; facilitated transport

Recommended Citations

Citations

  • Han, Y. (2018). Facilitated Transport Membranes for Carbon Capture from Flue Gas and H2 Purification from Syngas: From Membrane Synthesis to Process Design [Doctoral dissertation, Ohio State University]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=osu1543333780761185

    APA Style (7th edition)

  • Han, Yang. Facilitated Transport Membranes for Carbon Capture from Flue Gas and H2 Purification from Syngas: From Membrane Synthesis to Process Design. 2018. Ohio State University, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=osu1543333780761185.

    MLA Style (8th edition)

  • Han, Yang. "Facilitated Transport Membranes for Carbon Capture from Flue Gas and H2 Purification from Syngas: From Membrane Synthesis to Process Design." Doctoral dissertation, Ohio State University, 2018. http://rave.ohiolink.edu/etdc/view?acc_num=osu1543333780761185

    Chicago Manual of Style (17th edition)

osu1543333780761185
247
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This open access ETD is published by The Ohio State University and OhioLINK.