Table 1. Reaction Optimization and Control Experiments.
| entrya | cat. (mol %) | add. (mol %) | yieldb (%) | e.r.c |
|---|---|---|---|---|
| 1 | 4-BArF24 (10) | N(nBu)4-(R)-5 (20) | 37 | 75:25 |
| 2 | 4-BArF24 (10) | - | 60 | - |
| 3 | 4-OTf (10) | - | 19 | - |
| 4 | 4-OTf (10) | N(nBu)4-(R)-5 (20) | 19 | 50:50 |
| 5 | - | N(nBu)4-(R)-5 (20) | 8 | 51:49 |
| 6 | - | H-(R)-5 (20) | 12 | 51:49 |
| 7 | - | - | 12 | - |
| 8 | 4-BArF24 (10) | H-(R)-5 (20) | <5 | 53:47 |
| 9 | 4-BArF24 (10) | N(nBu)4-(S)-6 (20) | 23 | 69:31 |
| 10 | 4-BArF24 (10) | N(nBu)4-(S)-7 (20) | 35 | 76:24 |
| 11 | 4-BArF24 (10) | N(nBu)4-(S)-8 (20) | 46 | 86:14 |
| 12 | 4-BArF24 (10) | N(nBu)4-(S)-9 (20) | 69 | 85:15 |
| 13 | 4-BArF24 (10) | N(nBu)4-(S)-9 (10) | 34 | 48:52 |
| 14 | 4-BArF24 (10) | N(nBu)4-(S)-9 (30) | 54 | 82:18 |
| 15 | - | Na-(S)-9 (20) | 25 | 49:51 |
| 16 | 4-(S)-9 (10) | - | >95 | 88:12 |
| 17d | 4-(S)-9 (10) | - | >95 | 89:11 |
| 18d,e | 4-(S)-8 (10) | - | 94f | 93:7 |
| 19g,h | 4-(S)-8 (10) | - | 56f | 94.5:5.5 |
| 20g | 4-(S)-8 (5) | - | 32 | 93.5:6.5 |
| 21g | 4-(S)-8 (2) | - | 10 | 87:13 |
| 22d | - | H-(S)-8 (20) | 9 | 51:49 |
| 23d | - | - | 9 | - |
Reactions (Scheme 1) performed at 12.5/25 μmol scale using 10 equiv of cyclopentadiene (2) and the catalyst (cat.)/additive (add.) in the given amounts in toluene (100 mM).
Determined for endo-3a44 via 1H NMR spectroscopy using methyl 3,5-dinitrobenzoate as internal standard.
Determined for endo-3a via chiral HPLC.
50 mM concentration.
50 μmol scale.
Isolated yield of 3a (endo:exo >100:1).
12.5 mM concentration.
50 and 100 μmol scale.