Desulfurization of Transportation Fuels with Zeolites Under Ambient Conditions

American Association for the Advancement of Science (AAAS) - Tập 301 Số 5629 - Trang 79-81 - 2003
Ralph T. Yang1, Arturo J. Hernández‐Maldonado1, Frances H. Yang1
1Department of Chemical Engineering, University of Michigan, Ann Arbor, MI 48109, USA

Tóm tắt

Deep desulfurization of transportation fuels (gasoline, diesel, and jet fuels) is being mandated by U.S. and foreign governments and is also needed for future fuel cell applications. However, it is extremely difficult and costly to achieve with current technology, which requires catalytic reactors operated at high pressure and temperature. We show that Cu + and Ag + zeolite Y can adsorb sulfur compounds from commercial fuels selectively and with high sulfur capacities (by π complexation) at ambient temperature and pressure. Thus, the sulfur content was reduced from 430 to <0.2 parts per million by weight in a commercial diesel at a sorbent capacity of 34 cubic centimeters of clean diesel produced per gram of sorbent. This sulfur selectivity and capacity are orders of magnitude higher than those obtained by previously known sorbents.

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Tài liệu tham khảo

A. Avidan M. Cullen paper AM-01-55 presented at the National Petroleum and Refiners Association Annual Meeting Washington DC 18 to 20 March 2001.

B. C. Gates J. R. Katzer G. C. A. Schuit Chemistry of Catalytic Processes (McGraw-Hill New York 1979) chap. 5.

R. T. Yang Adsorbents: Fundamentals and Applications (Wiley New York 2003) chap. 10. This reference contains a detailed review of the literature of all commercial and nontraditional sorbents that have been tested as well as the different approaches for deep desulfurization of transportation fuels.

A. J. Hernández-Maldonado, R. T. Yang, Ind. Eng. Chem. Res.42, 123 (2003).

The calculations were performed at the Hartree-Fock and density functional theory level using effective core potentials ( 11 ). The restricted Hartree-Fock theory at the LanL2DZ level basis set ( 12 ) was used to determine the geometries and the adsorption bonding energies ( 8 ). Natural bond orbital analysis at the B3LYP/LanL2DZ level was used for studying the electron density distribution of the adsorption system ( 8 ). A cluster model was used to represent zeolite framework structure to which Ag + and Cu + cations were bonded.

A. Takahashi, F. H. Yang, R. T. Yang, Ind. Eng. Chem. Res.41, 2487 (2002).

The adsorber bed contained 1 to 2 g of zeolite and the feed flow rate was maintained at 0.5 cm 3 /min. Effluent (or eluent) samples were collected at regular intervals until saturation was reached and the samples were subsequently analyzed for sulfur-containing compounds with a gas chromatograph (GC) equipped with a flame photometric detector (FPD). The FPD was operated at a sensitivity (or detection limit) of 0.02 ppmw sulfur. Fourier transform infrared spectroscopy was used for analysis of aromatic and aliphatic contents by means of the C-H stretching bands.

S. C. Larson, A. Aylor, A. T. Bell, J. A. Reimer, J. Phys. Chem.98, 11533 (1994).

X. Ma, S. Lu, C. Song, Catal. Today77, 107 (2002).

Fuel Cells for Transportation 2001 Annual Report (U.S. Department of Energy Office of Transportation Technologies Washington DC 2001).

P. J. Hay, W. R. Wadt, J. Chem. Phys.82, 299 (1985).

T. V. Russo, R. L. Martin, P. J. Hay, J. Phys. Chem.99, 17085 (1995).

This work was funded by NSF and the U.S. Department of Energy. U.S. and foreign patents are pending.

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American Association for the Advancement of Science (AAAS)

Tập 301 Số 5629

79-81

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