Grantee Research Project Results
2000 Progress Report: Federal Demonstration Partnership (FDP) solid-catalyzed reactions in supercritical reaction media
EPA Grant Number: R826034Title: Federal Demonstration Partnership (FDP) solid-catalyzed reactions in supercritical reaction media
Investigators: Subramaniam, Bala
Institution: University of Kansas
EPA Project Officer: Aja, Hayley
Project Period: October 1, 1998 through September 30, 2001 (Extended to May 20, 2003)
Project Period Covered by this Report: October 1, 1999 through September 30, 2000
Project Amount: $125,000
RFA: Technology for a Sustainable Environment (1998) RFA Text | Recipients Lists
Research Category: Nanotechnology , Sustainable and Healthy Communities , Pollution Prevention/Sustainable Development
Objective:
The objectives of the research project are to: (1) develop a solid-acid catalyzed 1-butene/isobutane and skeletal isomerization process with enhanced catalyst activity and product selectivity; and (2) demonstrate the safe operation (characterized by stable catalyst activity and excellent temperature control) of solid catalyzed hydrogenations in supercritical CO2-based reaction media.Progress Summary:
The demonstration of extended butene conversion (80 percent) and C8 selectivity (~74 percent, with the alkylates constituting approximately 40 percent of the total C8 compounds) at a relatively mild pressure (80 bar at 568 K), low I/O ratio (5), and reasonable CO2 dilution (70 percent) is a significant advance over previous efforts. Our results clearly indicate that with rational design of catalyst, tailoring parameters such as acidity and pore structure, it should be possible to further enhance the C8 alkylates selectivity. Thus, CO2-based supercritical reaction mixtures offer an excellent opportunity in general for developing environmentally benign alternatives to conventional processes that employ mineral acids.
The equipment infrastructure and the insights provided by the foregoing results on how to operate an exothermic reaction in scCO2 with tight temperature control and stable catalyst activity pave the way for systematic fundamental investigations of fixed-bed hydrogenations of functional groups on supported catalysts. Clearly, such investigations are essential for rational design and scaleup of scCO2-based hydrogenations.
Future Activities:
Specific activities include: (1) the development of experimental and modeling tools that aid in the rational analysis, design, and operation of continuous sc phase reactors; (2) the optimization of the scCO2-based, fixed-bed hydrogenations on supported catalysts aimed at maximizing the selectivity of the desired product?this optimization will be based on systematic experimental and modeling studies that take into account the phase behavior of the reaction mixture, the intrinsic hydrogenation kinetics, temperature control, and catalyst deactivation issues; and (3) the optimization of the scCO2-based solid-acid alkylation process developed in our laboratory, aimed at demonstrating C8 alkylates selectivity that are comparable to those obtained with mineral acids. This optimization will be achieved via rational design of solid-acid catalysts (with controlled pore size and acid site density/accessibility) complemented by modeling studies based on a reliable knowledge of the intrinsic kinetics.Journal Articles on this Report : 3 Displayed | Download in RIS Format
Other project views: | All 28 publications | 9 publications in selected types | All 8 journal articles |
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Arunajatesan V, Subramaniam B, Hutchenson KW, Herkes FE. Fixed-bed hydrogenation of organic compounds in supercritical carbon dioxide. Chemical Engineering Science 2001;56(4):1363-1369. |
R826034 (2000) R826034 (2001) |
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Lyon CJ, Subramaniam B, Pereira CJ. Extended alkylate production on SiO2-supported Nafion at supercritical conditions.. Studies In Surface Sciences. 2001;139:221-228. |
R826034 (2000) |
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Subramaniam B. Enhancing the stability of porous catalysts with supercritical reaction media. Applied Catalysis A:General 2001;212(1-2):199-213. |
R826034 (2000) R826034 (2001) |
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Supplemental Keywords:
supercritical carbon dioxide, acid catalyst, hydrogenation, 1-butene/isobutane alkylation., RFA, Industry Sectors, Scientific Discipline, Sustainable Industry/Business, Chemical Engineering, cleaner production/pollution prevention, Environmental Chemistry, Manufacturing - NAIC 31-33, Sustainable Environment, Technology for Sustainable Environment, Environmental Engineering, Accommodation and Food Services - NAIC 72, Federal Demostration Program, aldehydes, cleaner production, environmentally conscious manufacturing, sustainable development, waste minimization, waste reduction, Federal Demonstration Partnership, solid-catalyzed reactions, catalysts, green process systems, alkylation reaction, isomerization, catalysis, pollution prevention, source reduction, supercritical reaction media, green chemistryRelevant Websites:
Progress and Final Reports:
Original AbstractThe perspectives, information and conclusions conveyed in research project abstracts, progress reports, final reports, journal abstracts and journal publications convey the viewpoints of the principal investigator and may not represent the views and policies of ORD and EPA. Conclusions drawn by the principal investigators have not been reviewed by the Agency.