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• W2000371325 abstract "The rhodium(I) complexes HRh(CO)[Ph2P(CH2)xSi(OMe)3]3 [1a,b(T0)3; a: x=3, b: x=6; T: T-type silicon atom, three oxygen neighbors] were sol–gel processed with the bifunctional cocondensation agent (MeO)3Si(CH2)6Si(OMe)3 (T–C6–T) and in a separate reaction also with three additional equivalents of the phosphine ligand Ph2P(CH2)xSi(OMe)3 [2a,b(T0)]. The resulting stationary phases 1a(Tn)3(Tn–C6–Tn)y, 1a(Tn)3[2a(Tn)]3(Tn–C6–Tn)y, and 1b(Tn)3[2b(Tn)]3(Tn–C6–Tn)y (n=0–3, number of Si–O–Si bonds; y: content of cocondensation agent) show a relatively narrow particle size distribution. The structural integrity of the rhodium complex 1 after the polycondensation was established by an EXAFS structure elucidation of the polysiloxane 1a(Tn)3. The obtained stationary phases proved to be efficient catalysts for the hydroformylation of 1-hexene in the presence of a wide variety of solvents in the interphase. Application of the materials containing non-coordinated ligands raised the selectivity toward hydroformylation up to 92% and the n/iso ratio to 14:1 with an average turnover number of 164 molsub molcat−1 h−1. Higher olefins than 1-hexene were also hydroformylated with catalyst D and similar turnover frequencies and selectivities were obtained. 31P CP/MAS NMR relaxation time studies (TPH, T1ρH) were carried out in the presence (interphase) or absence (stationary phase) of a swelling solvent to investigate the dynamic behavior of the catalytically active polymer 1a(Tn)3[2a(Tn)]3(Tn–C6–Tn)y. The highest mobility of the nonpolar reactive centers was achieved in nonpolar solvents like toluene, while more polar solvents like ethanol afforded the highest mobility of the overall polymer. (1H,31P) 2D WISE NMR experiments performed on the same material revealed a substantial decrease of the line width for the swollen polymer. 29Si CP/MAS NMR experiments revealed a high degree of cross-linking and a larger content of cocondensation agent than introduced before condensation." @default.
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• W2000371325 date "2000-06-01" @default.
• W2000371325 modified "2023-10-17" @default.
• W2000371325 title "Supported organometallic complexes. Part XX. Hydroformylation of olefins with rhodium(I) hybrid catalysts" @default.
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• W2000371325 doi "https://doi.org/10.1016/s1381-1169(00)00038-8" @default.
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