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Desulfurization with transition metal catalysts: scope and mechanism of cleaving carbon-sulfur and carbon-nitrogen bonds with subvalent organotransition-metal complexes: Final technical report, September 27, 1981-December 31, 1983

Technical Report ·
OSTI ID:6989416

Our fundamental interest in this research is to understand the reaction mechanisms whereby lower valent transition-metal complexes bring about the cleavage of relatively weak pi- and sigma- covalent bonds. Such a long-range physical-chemical investigation should put the effects of the metal's electronic configuration, the ligands on the metal and the nature of the solvent on a more rational basis. As an ultimate result, a more systematic approach to varying the reactivity of transition-metal catalysts ought to be attainable. The design of new catalytic systems, in general, and of new catalysts for heteroatom removal, in particular, should profit from our studies. The specific rationale of our investigation has been to choose a variety of organosulfur and organonitrogen compounds, with which to evaluate the desulfurizing and denitrogenating action of low-valent transition metal complexes. Such organic compounds were selected for study, because they closely resemble the kinds of sulfur- and nitrogen-containing structures occurring in coal or coal-liquids themselves. As model compounds, we have examined aryl mercaptans, sulfides and disulfides, aromatic sulfur heterocycles (diobenzothiophenes, thianthrene, phenothiazine and phenoxathiin), pyrrole derivatives and benzopyridines. Once the most favorable choice of experimental variables is attained with the model nitrogen- or sulfur-containing compound, then the heteroatom-removing reagent is applied to an actual coal liquid. Results on desulfurization and denitrogenation of model organic compounds and coal liquids are reviewed. 27 refs., 6 tabs.

Research Organization:
State Univ. of New York, Binghamton (USA). Dept. of Chemistry
DOE Contract Number:
FG22-81PC40782
OSTI ID:
6989416
Report Number(s):
DOE/PC/40782-T7; ON: DE87002559
Country of Publication:
United States
Language:
English