High-Capacity Sulfur Dioxide Absorbents for Diesel Emissions Control
High capacity sulfur dioxide absorbents based on manganese oxide octahedral molecular sieves (OMS) have been identified. These materials are based on MnO6 octahedra sharing faces and edges to form various tunnel structures (2x2, 2x3, 2x4, 3x3) differentiated by the number of octahedra on a side. The SO2 capacities of these materials, measured at 325 C with a feed containing 250 ppmv SO2 in air, are as high as 70wt% (wt/wt), remarkably higher than conventional metal oxide-based SO2 absorbents. Among the OMS materials the 2x2 member, cryptomelane, exhibits the highest capacity and adsorption rate. Its SO2 absorption behavior has been further characterized as a function of temperature, space velocity, and feed composition. The dominant pathway for SO2 absorption is through the oxidation of SO2 to SO3 by Mn4+ followed by SO3 reaction with Mn2+ to form MnSO4. Absorption can occur in the absence of gas phase oxygen, with a moderate loss in overall capacity. The inclusion of reducible gases NO and CO in the feed does not reduce SO2 capacity. The absorption capacity decreases at high space velocity and lower absorption temperature, indicating the important role of diffusion of sulfate from the surface to the bulk of the material in order to reach full capacity. A color change of cryptomelane from black to yellow-brown after SO2 absorption can be used as an indicator of absorption progress. Cryptomelane can be synthesized using MnSO4 as a reagent. Therefore, after full SO2 absorption the product MnSO4 can be re-used as raw material for a subsequent cryptomelane synthesis. Cryptomelane has a similarly high capacity toward SO3, therefore it can be used for removal of all SOx species generated from a variety of combustion sources. Cryptomelane may find application as a replaceable absorbent for the removal of SOx from diesel truck exhaust, protecting downstream emissions control devices such as particulate filters and NOx traps.
- Research Organization:
- Pacific Northwest National Lab., Richland, WA (US)
- Sponsoring Organization:
- US Department of Energy (US)
- DOE Contract Number:
- AC05-76RL01830
- OSTI ID:
- 15016362
- Report Number(s):
- PNNL-SA-42474; IECRED; TRN: US200513%%171
- Journal Information:
- Industrial and Engineering Chemistry Research, Vol. 44, Issue 1; Other Information: PBD: 5 Jan 2005; ISSN 0888-5885
- Country of Publication:
- United States
- Language:
- English
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