Table 2. Single and double asymmetric homoallylic alcohol–imine coupling reactions en route to chiral piperidines.
entry | homoallylic alcohol | imine | 1,5-aminoalcohola | yield (%) | dr | piperidineb(yield) |
---|---|---|---|---|---|---|
1 | 83 | 24:1 | ||||
2 | 124 | 75 | 20:1 | |||
3 | 124 | 127 | 61 | 25:4:1 | ||
4 | ent-124 | 76 | ≥50:1 | |||
5 | 124 | 88 | 35:4:1 |
Reaction conditions for cross coupling: imine (1 eq), Ti(Oi-Pr)4 (1.5 eq), c-C5H9MgCl (3.0 eq), Et2O (−60 to −30 °C), then add alkoxide (1.5 eq) (−40 to 0 °C or rt).
Reaction conditions for cyclization: For 126 - 2-NsCl, Et3N, DMAP, CH2Cl2, rt. For 128 -MsCl, Et3N, CH2Cl2, rt. R = CH(Ph)CH2OMe. For 131 and 134 - 1) H2 (1 atm), Pd(OH)2, AcOH/MeOH (1:10 v/v), rt, 2) 2-NsCl, Et3N, DMAP, CH2Cl2, 0 °C to rt, 3) PPh3, DIAD, THF, rt.