Cooperative Tandem Catalysis by an Organometallic Complex and a Metalloenzyme

Cooperative Tandem Catalysis by an Organometallic Complex and a Metalloenzyme
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DOI:
10.1002/anie.201305778
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发表时间:
2014-01-07
影响因子:
16.6
通讯作者:
Hartwig, John F.
Hartwig, John F.
中科院分区:
化学1区
文献类型:
--
作者:
Denard, Carl A.;Huang, Hua;Hartwig, John F.

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虽然化学催化剂和酶催化剂已经结合在一起,但有机金属催化剂和金属酶协同作用产生的产物,不能单独使用催化剂或通过两种催化剂的顺序反应产生相当的产量,还没有报道。这样的反应很难实现,部分原因是这些催化剂的作用环境通常是不同的。本文证明了两类催化剂在同一体系中协同反应。复分解催化剂和P450酶的组合导致烯烃的动态平衡和交叉复分解产物的选择性环氧化。这些结果显示了将这两类催化剂结合起来用于合成转化的潜力。
Although chemical and enzymatic catalysts have been combined, reactions in which an organometallic catalyst and a metalloenzyme work cooperatively to create products, which cannot be generated with either catalyst alone or in comparable yields by sequential reactions of the two catalysts, have not been reported. Such reactions are challenging to achieve, in part because the milieu in which these catalysts operate are typically different. Herein, two classes of catalysts are demonstrated to react cooperatively in the same system. Combination of a metathesis catalyst and a P450 enzyme lead to a dynamic equilibration of alkenes and a selective epoxidation of the cross-metathesis products. These results show the potential of combining the two classes of catalysts for synthetic transformations.