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The diacetate complexes trans -[Ru(κ 1 -OAc) 2 (PPh 3 ) 2 (NN)] (NN = ethylenediamine (en) ( 1 ), 2-(aminomethyl)pyridine (ampy) ( 2 ), 2-(aminomethyl)pyrimidine (ampyrim) ( 3 )) have been isolated in 76-88% yield by reaction of [Ru(κ 2 -OAc) 2 (PPh 3 ) 2 ] with the corresponding nitrogen ligands. The ampy-type derivatives 2 and 3 undergo isomerization to the thermodynamically most stable cationic complexes [Ru(κ 1 -OAc)(PPh 3 ) 2 (NN)]OAc ( 2a and 3a ) and cis -[Ru(κ 1 -OAc) 2 (PPh 3 ) 2 (NN)] ( 2b and 3b ) in methanol at RT. The trans -[Ru(κ 1 -OAc) 2 (P 2 ) 2 ] (P 2 = dppm ( 4 ), dppe ( 5 )) compounds have been synthesized from [Ru(κ 2 -OAc) 2 (PPh 3 ) 2 ] by reaction with the suitable diphosphine in toluene at 95 °C. The complex cis -[Ru(κ 1 -OAc) 2 (dppm)(ampy)]( 6 ) has been obtained from [Ru(κ 2 -OAc) 2 (PPh 3 ) 2 ] and dppm in toluene at reflux and reaction with ampy. The derivatives trans -[Ru(κ 1 -OAc) 2 P 2 (NN)] ( 7 - 16 ; NN = en, ampy, ampyrim, 8-aminoquinoline; P 2 = dppp, dppb, dppf, ( R )-BINAP) can be easily synthesized from [Ru(κ 2 -OAc) 2 (PPh 3 ) 2 ] with a diphosphine and treatment with the NN ligands at RT. Alternatively these compounds have been prepared from trans -[Ru(OAc) 2 (PPh 3 ) 2 (NN)] by reaction with the diphosphine in MEK at 50 °C. The use of ( R )-BINAP affords trans -[Ru(κ 1 -OAc) 2 (( R )-BINAP)(NN)] (NN = ampy ( 11 ), ampyrim ( 15 )) isolated as single stereoisomers. Treatment of the ampy-type complexes 8 - 15 with methanol at RT leads to isomerization to the cationic derivatives [Ru(κ 2 -OAc)P 2 (NN)]OAc ( 8a - 15a ; NN = ampy, ampyrim; P 2 = dppp, dppb, dppf, ( R )-BINAP). Similarly to 2 , the dipivalate trans -[Ru(κ 1 -OPiv) 2 (PPh 3 ) 2 (ampy)] ( 18 ) is prepared from [Ru(κ 2 -OPiv) 2 (PPh 3 ) 2 ] ( 17 ) and ampy in CHCl 3 . The pincer acetate [Ru(κ 1 -OAc)(CNN OMe )(PPh 3 ) 2 ] ( 19 ) has been synthesized from [Ru(κ 2 -OAc) 2 (PPh 3 ) 2 ] and HCNN OMe ligand in 2-propanol with NEt 3 at reflux. In addition, the dppb pincer complexes [Ru(κ 1 -OAc)(CNN)(dppb)] (CNN = AMTP ( 20 ), AMBQ Ph ( 21 )) have been obtained from [Ru(κ 2 -OAc) 2 (PPh 3 ) 2 ], dppb, and HAMTP or HAMBQ Ph with NEt 3 , respectively. The acetate NN and pincer complexes are active in transfer hydrogenation with 2-propanol and hydrogenation with H 2 of carbonyl compounds at S/C values of up to 10000 and with TOF values of up to 160000 h -1 .

organometallics

Preparation of Neutral trans - cis [Ru(O2CR)2P2(NN)], Cationic [Ru(O2CR)P2(NN)](O2CR) and Pincer [Ru(O2CR)(CNN)P2] (P = PPh3, P2 = diphosphine) Carboxylate Complexes and their Application in the Catalytic Carbonyl Compounds Reduction