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Desulfurization with transition metal catalysts

Technical Report ·
OSTI ID:5649840
The principal objective of this research is to uncover new reagents and catalysts for upgrading coal-derived fuels by removing undesirable organosulfur, organonitrogen and, if feasible, oxygen components. During the sixth quarter of this two-year grant the following studies were continued: (a) evaluation of the combined desulfurizing action on SRC liquids of nickel salts and metal hydrides, especially when the reactants are deposited on or attached to inorganic or organic supports; (b) assessment of the efficacy of the solid support in enhancing the desulfurizing action of the subvalent nickel; (c) devising an effective and safe way of maintaining desulfurization columns of such solid supports at 40 to 100/sup 0/C for extended periods; and (d) carrying out exploratory work on denitrogening model organic compounds. The following progress had been made: (a) after much experimentation, a heated, packed percolation column containing the nickel-based desulfurization agent has been devised, which permits the efficient passage of SRC liquids in reasonable periods of time; (b) evaluations continue of combinations of poly(40-vinylpyridine) and alumina as the solid support, and modest desulfurization (20%) of the SRC liquid has been observed; (c) various pretreatments of poly(4-vinylpyridine) with sodium diethylaluminum hydride aim at affixing the reducing agent to the polymer by hydralumination of the pyridine nucleus, thereby immobilizing the reductant and eventually the nickel reagent; (d) regeneration of nickelsulfide-containing columns by treatment with acetylacetone alone is not feasible, but stronger acids appear promising; and (e) although NaAlEt/sub 2/H/sub 2/ and various salts (Ti, Cr, Ni, Mo) were unreactive toward N-benzylcarbazole, a combination of lithium metal and titanium or nickel salts did cleave C-N bonds to form carbazole and some ammonia.
Research Organization:
State Univ. of New York, Binghamton (USA). Dept. of Chemistry
DOE Contract Number:
FG22-81PC40782
OSTI ID:
5649840
Report Number(s):
DOE/PC/40782-T5; ON: DE83013607
Country of Publication:
United States
Language:
English