Table 4. Reductive Amination Approach to (4R)-9ba.
entry | (b) step 1 | (b) step 2 | (b) solvent | (4R)-9b:(4S)-9b | yield of (4R)-9b (%) |
---|---|---|---|---|---|
1 | 2.5 equiv Ti(OPri)4 | 1.3 equiv NaBH3CN | MeOH | 1:1 | |
2 | 0.6 equiv TiCl4 | 0.2 equiv Pd/C, H2 | MeOH | 1:1 | |
3 | 0.6 equiv TiCl4 | 0.2 equiv PtO2, H2 | MeOH | 2:1 | 30 |
4 | 0.6 equiv TiCl4 | 0.2 equiv PtO2, H2 | CH2Cl2 | 4:1 | 50 |
5 | 0.7 equiv TiCl4 | 1.1 equiv BH3 (1 M THF) | CH2Cl2 | 1:1 | |
6 | 0.7 equiv TiCl4 | 1.1 equiv BH3·SMe2 | CH2Cl2 | 6:1 | 70 |
7 | 1.1 equiv Ti(OEt)4 | 1.1 equiv BH3·SMe2 | CH2Cl2 | 1:1 | |
8 | 0.6 equiv TiCl4 and 0.6 equiv Ti(OPri)4 | 1.1 equiv BH3·SMe2 | CH2Cl2 | 8:1 | 78 |
Reagents and conditions. (a) step 1: TFA, CH2Cl2, rt, 1 h, 93% yield; step 2: 3,5-di-tert-butylcyclohexa-3,5-diene-1,2-dione, Dowex-50WX8–200 resin, MeOH, 90% yield; (b) step 1 :2 equiv t-BuNH2; step-2: rt 16 h.