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Selective transformation of carbonyl ligands to organic molecules

Technical Report ·
OSTI ID:6716864

Three objectives of our studies on the catalytic hydrosilation of organo-transition metal acyl complexes have been attained. First, efficient catalysts and near optimal reaction conditions now supersede our previous procedures using (PPh{sub 3}){sub 3}RhCl. Manganese acyl compounds L(CO){sub 4}MnCOR (L = CO/R = Me, Ph; L = PPh{sub 3}, PEt{sub 3}/R = Me) as catalysts (0.1 to 10%) promote addition of R{prime}{sub 2}SiH{sub 2} (R{prime} = Et, Ph) and R{prime}{sub 3}SiH (R{prime}{sub 3} = Et{sub 3}, Me{sub 2}Ph) across FpCOR{double prime} (R{double prime} = Me, Ph), our test substrates. Second, diastereo-selective hydrosilylation ((PPh{sub 3}){sub 3}RhCl catalysis/R{prime}{sub 2}SiH{sub 2}) of chiral Fe and Ru acetyl complexes Cp(L)(CO)M-COCH{sub 3} (L = P(OMe){sub 3}, PEt{sub 3}, PPh{sub 3}) has been achieved. Studies in progress focus on comparing this diastereoselectivity with that observed in generating corresponding {alpha}-alkoxyethyl complexes from reduction of Cp(L)(CO)M = C(OEt)CH{sub 3}{sup +} and on minimizing the subsequent conversion of the resulting siloxyethyl complexes to their vinyl derivatives, Cp(L)(CO)M {minus} CH = CH{sub 2}. Third, coupling hydrosilylation and subsequent carbonylation steps has been achieved using (CO){sub 5}Mn acyl complexes. Satisfactory progress also is being made on the hydrosilylation (catalytic-potentially drastereoselective) then carbonylation of ({eta}{sup 5}-indenyl)Ru acetyl compounds, In(L)(CO)Ru--COCH{sub 3}.

Research Organization:
Rensselaer Polytechnic Inst., Troy, NY (USA). Dept. of Chemistry
Sponsoring Organization:
DOE/ER
DOE Contract Number:
FG02-86ER13617
OSTI ID:
6716864
Report Number(s):
DOE/ER/13617-4; ON: DE90015387
Country of Publication:
United States
Language:
English