STUDY OF SOLVENT AND CATALYST INTERACTIONS IN DIRECT COAL LIQUEFACTION
There are several aspects of the Direct Coal Liquefaction process which are not fully understood and which if better understood might lead to improved yields and conversions. Among these questions are the roles of the catalyst and the solvent. While the solvent is known to act by transfer of hydrogen atoms to the free radicals formed by thermal breakdown of the coal in an uncatalyzed system, in the presence of a solid catalyst as is now currently practiced, the yields and conversions are higher than in an uncatalyzed system. The role of the catalyst in this case is not completely understood. DOE has funded many projects to produce ultrafine and more active catalysts in the expectation that better contact between catalyst and coal might result. This approach has met with limited success probably because mass transfer between two solids in a fluid medium i.e. the catalyst and the coal, is very poor. It is to develop an understanding of the role of the catalyst and solvent in Direct Liquefaction that this project was initiated. Specifically it was of interest to know whether direct contact between the coal and the catalyst was important. By separating the solid catalyst in a stainless steel basket permeable to the solvent but not the coal in the liquefaction reactor, it was shown that the catalyst still maintains a catalytic effect on the liquefaction process. There is apparently transfer of hydrogen atoms from the catalyst through the basket wall to the coal via the solvent. Strong hydrogen donor solvents appear to be more effective in this respect than weak hydrogen donors. It therefore appears that intimate contact between catalyst and coal is not a requirement, and that the role of the catalyst may be to restore the hydrogen donor strength to the solvent as the reaction proceeds. A range of solvents of varying hydrogen donor strength was investigated. Because of the extensive use of thermogravimetric analysis in this laboratory in was noted that the peak temperature for volatile evolution from coal was a reliable measure of coal rank. Because of this observation, a wide variety of coals of a wide range of ranks was investigated. It was shown in this work that measuring the peak temperature for volatile evolution was quite a precise indicator of rank and correlated closely wit the rank values obtained by measuring vitrinite reflectance, a more difficult measurement to make. This prompted the desire to know the composition of the volatile materials evolved as a function of coal rank. This was then measured by coupling a TGA to a mass spectrometer using laser activation and photoionization detection TG-PI-MS. The predominant species in volatiles of low rank coal turned out to be phenols with some alkenes. As the rank increases, the relative amount of alkenes and aromatic hydrocarbons increases and the oxygenated species decrease. It was shown that these volatiles were actually pyrolitic products and not volatilization products of coal. Solvent extraction experiments coupled with TG-PI-MS indicates that the low oiling and more extractable material are essentially similar in chemical types to the non-extractable portions but apparently higher molecular weight and therefor less extractable.
- Research Organization:
- National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV, and Albany, OR (United States)
- Sponsoring Organization:
- US Department of Energy (US)
- DOE Contract Number:
- FG26-97FT97264
- OSTI ID:
- 791852
- Report Number(s):
- FG26-97FT97264-03; TRN: US200204%%193
- Resource Relation:
- Other Information: PBD: 1 Jan 2000
- Country of Publication:
- United States
- Language:
- English
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STUDY OF SOLVENT AND CATALYST INTERACTIONS IN DIRECT COAL LIQUEFACTION
STUDY OF SOLVENT AND CATALYST INTERACTIONS IN DIRECT COAL LIQUEFACTION