Carbon Dioxide Separation with Novel Microporous Metal Organic Frameworks

Willis, Richard ; Benin, Annabelle ; Low, John ; Venimadhavan, Ganesh ; Faheem, Syed ; Lesch, David ; Matzger, Adam ; Snurr, Randy

UOP LLC

关键词: Desorption;    Raman Spectroscopy;    Surface Area;    X-Ray Diffractometers;    Carbon Dioxide;   

DOI  :  10.2172/1001228
RP-ID  :  None
RP-ID  :  FG26-04NT42121
RP-ID  :  1001228

美国|英语

来源: UNT Digital Library

【 摘 要 】

The goal of this program was to develop a low cost novel sorbent to remove carbon dioxide from flue gas and gasification streams in electric utilities. Porous materials named metal-organic frameworks (MOFs) were found to have good capacity and selectivity for the capture of carbon dioxide. Several materials from the initial set of reference MOFs showed extremely high CO{sub 2} adsorption capacities and very desirable linear isotherm shapes. Sample preparation occurred at a high level, with a new family of materials suitable for intellectual property protection prepared and characterized. Raman spectroscopy was shown to be useful for the facile characterization of MOF materials during adsorption and especially, desorption. Further, the development of a Raman spectroscopic-based method of determining binary adsorption isotherms was initiated. It was discovered that a stronger base functionality will need to be added to MOF linkers in order to enhance CO{sub 2} selectivity over other gases via a chemisorption mechanism. A concentrated effort was expended on being able to accurately predict CO{sub 2} selectivities and on the calculation of predicted MOF surface area values from first principles. A method of modeling hydrolysis on MOF materials that correlates with experimental data was developed and refined. Complimentary experimental data were recorded via utilization of a combinatorial chemistry heat treatment unit and high-throughput X-ray diffractometer. The three main Deliverables for the project, namely (a) a MOF for pre-combustion (e.g., IGCC) CO{sub 2} capture, (b) a MOF for post-combustion (flue gas) CO{sub 2} capture, and (c) an assessment of commercial potential for a MOF in the IGCC application, were completed. The key properties for MOFs to work in this application - high CO{sub 2} capacity, good adsorption/desorption rates, high adsorption selectivity for CO{sub 2} over other gases such as methane and nitrogen, high stability to contaminants, namely moisture, and easy regenerability, were all addressed during this program. As predicted at the start of the program, MOFs have high potential for CO{sub 2} capture in the IGCC and flue gas applications.