Faculty of Science, Charles University in Prague, Hlavova 2030, 12843 Prague 6, Czech Republic.
Faraday Discuss. 2019 Dec 2;220(0):58-70. doi: 10.1039/c9fd00038k.
Bambusuril macrocycles have high affinity towards anions (X-) such as PF6- and SbF6- or BF4- and ClO4-. Therefore, addition of bambusurils to reaction mixtures containing these anions effectively removes the free anions from the reaction process. Hence, comparing reactions with and without addition of bambusurils can demonstrate whether the anions actively participate in the reaction mechanism or not. We show this approach for gold(i) mediated addition of methanol to an alkyne. The reaction mechanism can proceed via monoaurated intermediates (e.g., in catalysis with [(IPr)AuX]) or via diaurated intermediates (e.g., in catalysis with [(PPh3)AuX]). We show that anions X- slightly affect the reaction rates, however the effect stays almost the same even after their encapsulation in the cavity of bambusurils. We also demonstrate that X- affects the overall reaction rate in the very same way as the reaction rate of the protodeauration step. All results are consistent with the indirect effect of X- by the acidity of the conjugated acid HX on the rate-determining step. There is no evidence that a direct involvement of X- would affect the reaction rate.
竹节菌素大环对阴离子(如 PF6- 和 SbF6- 或 BF4- 和 ClO4-)具有高亲和力。因此,将竹节菌素添加到含有这些阴离子的反应混合物中,可以有效地将游离阴离子从反应过程中去除。因此,比较添加和不添加竹节菌素的反应可以证明阴离子是否积极参与反应机制。我们以金(i)介导的甲醇与炔烃加成反应为例展示了这种方法。反应机制可以通过单金中间体(例如,在 [(IPr)AuX] 的催化下)或通过二金中间体(例如,在 [(PPh3)AuX] 的催化下)进行。我们表明,阴离子 X- 会略微影响反应速率,但即使将其封装在竹节菌素的空腔中,其影响几乎保持不变。我们还证明,X- 以与原脱金步骤的反应速率相同的方式影响总反应速率。所有结果都与 X- 通过共轭酸 HX 的酸度对速率决定步骤的间接影响一致。没有证据表明 X- 的直接参与会影响反应速率。