Carbon Dioxide Removal from Flue Gas Using Microporous Metal Organic Frameworks

Lesch, David A

关键词: FLUE GAS;    AIR POLLUTION CONTROL;    CARBON DIOXIDE;    MATERIALS RECOVERY;    POROUS MATERIALS;    FOSSIL-FUEL POWER PLANTS;    COAL;    ADSORBENTS;    MATERIALS TESTING;    MOLECULAR MODELS;   

DOI  :  10.2172/1003992
RP-ID  :  None
PID  :  OSTI ID: 1003992
Others  :  TRN: US201105%%943

美国|英语

来源: SciTech Connect

【 摘 要 】

UOP LLC, a Honeywell Company, in collaboration with Professor Douglas LeVan at Vanderbilt University (VU), Professor Adam Matzger at the University of Michigan (UM), Professor Randall Snurr at Northwestern University (NU), and Professor Stefano Brandani at the University of Edinburgh (UE), supported by Honeywell's Specialty Materials business unit and the Electric Power Research Institute (EPRI), have completed a three-year project to develop novel microporous metal organic frameworks (MOFs) and an associated vacuum-pressure swing adsorption (vPSA) process for the removal of CO{sub 2} from coal-fired power plant flue gas. The project leveraged the team's complementary capabilities: UOP's experience in materials development and manufacturing, adsorption process design and process commercialization; LeVan and Brandani's expertise in high-quality adsorption measurements; Matzger's experience in syntheis of MOFs and the organic components associated with MOFs; Snurr's expertise in molecular and other modeling; Honeywell's expertise in the manufacture of organic chemicals; and, EPRI's knowledge of power-generation technology and markets. The project was successful in that a selective CO{sub 2} adsorbent with good thermal stability and reasonable contaminant tolerance was discovered, and a low cost process for flue gas CO{sub 2} capture process ready to be evaluated further at the pilot scale was proposed. The team made significant progress toward the current DOE post-combustion research targets, as defined in a recent FOA issued by NETL: 90% CO{sub 2} removal with no more than a 35% increase in COE. The team discovered that favorable CO{sub 2} adsorption at more realistic flue gas conditions is dominated by one particular MOF structure type, M/DOBDC, where M designates Zn, Co, Ni, or Mg and DOBDC refers to the form of the organic linker in the resultant MOF structure, dioxybenzenedicarboxylate. The structure of the M/DOBDC MOFs consists of infinite-rod secondary building units bound by DOBDC resulting in 1D hexagonal pores about 11 angstroms in diameter. Surface areas range from 800 to 1500 sq m/g for the different MOFs. Mg/DOBDC outperformed all MOF and zeolite materials evaluated to date, with about 25 wt% CO{sub 2} captured by this MOF at flue gas conditions ({approx}0.13 atm CO{sub 2} pressure, 311K). In simulated flue gas without oxygen, the zero-length (ZLC) system was very useful in quickly simulating the effect of long term exposure to impurities on the MOFs. Detailed adsorption studies on MOF pellets have shown that water does not inhibit CO{sub 2} adsorption for MOFs as much as it does for typical zeolites. Moreover, some MOFs retain a substantial CO{sub 2} capacity even with a modest water loading at room temperature. Molecular modeling was a key activity in three areas of our earlier DOE/NETL-sponsored MOF-based research on CC. First, the team was able to effectively simulate CO{sub 2} and other gas adsorption isotherms for more than 20 MOFs, and the knowledge obtained was used to help predict new MOF structures that should be effective for CO{sub 2} adsorption at low pressure. The team also showed that molecular modeling could be utilized to predict the hydrothermal stability of a given MOF. Finally, the team showed that low moisture level exposure actually enhanced the CO{sub 2} adsorption performance of a particular MOF, HKUST-1.