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Title: Simultaneous SO{sub 2}/No{sub x} abatement using zeolite-supported copper. Progress report, October 1--December 31, 1995

Abstract

Electron paramagnetic resonance (EPR) spectroscopy has been used to investigate the nature of copper ions supported on oxides and on zeolites. The results show that, unfortunately, EPR may not be a very useful predictor of the catalytic activity of supported copper catalysts.

Authors:
;
Publication Date:
Research Org.:
Clark Atlanta Univ., GA (United States)
Sponsoring Org.:
USDOE Assistant Secretary for Fossil Energy, Washington, DC (United States)
OSTI Identifier:
665879
Report Number(s):
DOE/MT/92017-03
ON: DE98057964; BR: AA1525150; TRN: AHC29819%%33
DOE Contract Number:
FG22-92MT92017
Resource Type:
Technical Report
Resource Relation:
Other Information: PBD: [1995]
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 01 COAL, LIGNITE, AND PEAT; PROGRESS REPORT; COMBINED SOXNOX PROCESSES; CATALYSTS; ELECTRON SPIN RESONANCE; PERFORMANCE; COPPER; CATALYTIC EFFECTS; ZEOLITES; SILICON OXIDES

Citation Formats

Mitchell, M.B., and White, M.G. Simultaneous SO{sub 2}/No{sub x} abatement using zeolite-supported copper. Progress report, October 1--December 31, 1995. United States: N. p., 1995. Web. doi:10.2172/665879.
Mitchell, M.B., & White, M.G. Simultaneous SO{sub 2}/No{sub x} abatement using zeolite-supported copper. Progress report, October 1--December 31, 1995. United States. doi:10.2172/665879.
Mitchell, M.B., and White, M.G. Sun . "Simultaneous SO{sub 2}/No{sub x} abatement using zeolite-supported copper. Progress report, October 1--December 31, 1995". United States. doi:10.2172/665879. https://www.osti.gov/servlets/purl/665879.
@article{osti_665879,
title = {Simultaneous SO{sub 2}/No{sub x} abatement using zeolite-supported copper. Progress report, October 1--December 31, 1995},
author = {Mitchell, M.B. and White, M.G.},
abstractNote = {Electron paramagnetic resonance (EPR) spectroscopy has been used to investigate the nature of copper ions supported on oxides and on zeolites. The results show that, unfortunately, EPR may not be a very useful predictor of the catalytic activity of supported copper catalysts.},
doi = {10.2172/665879},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Sun Dec 31 00:00:00 EST 1995},
month = {Sun Dec 31 00:00:00 EST 1995}
}

Technical Report:

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  • A flow reactor is being constructed at Georgia Tech for the NO decomposition reaction. The reactor is partially complete with the construction of a flow meter/controller system and a temperature controller system in place now. The stainless steel reactor tube and the furnace have been fabricated and fit to the sub-assembly containing the temperature control devices. The reactor sampling system is under fabrication. The authors plan to purchase a GC-MS to determine the composition of the exit gas. They have used Raman spectroscopy to characterize Zeolite A, a cobalt ethylenediamine complex, Co(en){sub 3}Cl{sub 3}, and Zeolite A impregnated with themore » cobalt complex. The Raman spectra from 1,700--100 cm{sup {minus}1} are shown.« less
  • We have made progress in characterizing a Cu-exchanged ZSM-5 for NO decomposition activity. Additionally, we are pursuing the impregnation of alumina with vanadium and copper and studying the adsorption and reaction of SO{sub 2} on these catalysts.
  • The proposed research seeks to advance/improve current flue gas cleanup catalyst technology by modifying promising copper-exchanged zeolite NO decomposition catalysts which reduce NO to elemental nitrogen and oxygen in the absence of an added reducing gas. The authors believe that this approach has great potential. Copper on alumina has been investigated by the Pittsburgh Energy Technology Center (PETC) as a NO{sub x}/SO{sub 2} abatement catalyst. Copper on alumina acts as a sorbent for SO{sub 2}, forming a surface sulfate upon adsorption in an oxygen-containing atmosphere, and as a catalyst for selective catalytic reduction (SCR) of NO{sub x} using ammonia; bothmore » CuO and CuSO{sub 4} on the surfaces of these materials are active SCR catalysts. SO{sub 2} adsorption in the PETC studies was carried out at 673K, a temperature well within the range for active NO decomposition by the Cu-ZSM-5 catalyst. The authors believe that by beginning with a material which decomposes NO without needing an added reducing gas, they will be able to design a catalyst which will act as a regenerable NO{sub x}/SO{sub 2} abatement catalyst which does not need ammonia to accomplish NO{sub x} reduction, and which will accomplish SO{sub 2} abatement by adsorption, similar to the copper on alumina catalyst. Coupled with a SO{sub 2} oxidation catalyst, this successful system will be able to remove both NO{sub x} and SO{sub 2} from flue gases with no added reducing agent and no waste.« less
  • We have significantly improved on our earlier results with a copper-impregnated alumina, obtaining reproducible results for the impregnation procedure and linear behavior with solution concentration of the precursor. The copper acetylacetonate precursor is adsorbed molecularly onto the alumina surface, with no noticeable decomposition. The adsorbed complex appears to form layers on the alumina surface, similar to results found using the same complex with a silica substrate. The materials start out as light blue powders, and after oxidation are light green. Using infrared spectroscopy, we have examined the in situ adsorption and oxidation of SO{sub 2} on the oxidized sorbent, whichmore » is dispersed copper oxide supported on aluminum oxide, and have observed that the initial species formed correspond to aluminum sulfate and aluminum sulfate. The sulfate is formed at temperatures much lower than similar experiments studying SO{sub 2} adsorption on alumina and sodium-doped alumina. As a result of oxidation, the adsorbed sulfur species, which begin as aluminum sulfate and sulfate, are converted to copper sulfate.« less
  • The bulk of the results from this project, besides being found in the research reports, are in the form of two theses presented for advanced degrees by two different students at two different institutions. Francis E. Porbeni is a Master`s Degree student in Chemistry at Clark Atlanta University and has prepared his Master`s Thesis entitled Simultaneous SO{sub 2} Oxidation and NO Decomposition over Copper Oxide on {gamma}-Alumina Catalysts: An Infrared Diffuse Reflectance Study. Sumit Rao, a Ph.D. student in Chemical Engineering at the Georgia Institute of Technology has defended his thesis entitled Role of Copper Ensemble Size in Silica andmore » Zeolite Supported Catalysts for Nitric Oxide Decomposition. These two documents, which will be forwarded when final copies are available, provide the details of the bulk of the research accomplished over the duration of this project. These two documents are summarized, and other results from the project are given.« less