使用设计的氧化酶-氧化酶互利系统进行非对称级联反应
Da Yu1,2, Jian-Bo Wang1,2, Manfred T Reetz3,4
1Key Laboratory of Phytochemistry R&D of Hunan Province, College of Chemistry and Chemical Engineering , Hunan Normal University , 410081 Changsha , People's Republic of China.
Journal of the American Chemical Society
|March 29, 2019
概括
使用P450酶的新型生物催化系统从3-酸中产生 (R) - 甘醇. 这种系统可回收过氧化,提高单合成的安全性和效率.
科学领域:
- 生物催化
- 酶工程
- 有机合成
背景情况:
- 开发高效的生物催化级联对于可持续的化学合成至关重要.
- P450酶具有多功能催化作用,但需要对H2O2等反应性中间体进行谨慎管理.
研究的目的:
- 为生物催化级联设计一个P450单氧化酶-过氧化酶系统.
- 从碳酸中实现 (R) - 甘醇及其衍生物的酶选择性合成.
主要方法:
- 使用P450单氧酶 (P450-BM3) 和P450过氧酶 (OleTJE) 构建生物催化级联.
- 针对 P450-BM3 的定向演化,以对烯中间体进行反选择性环氧化.
- 使用环氧化酶 (ANEH) 进行水解环开放.
主要成果:
- 建立了一个新的P450互利系统,使得H2O2在现场回收.
- 在合成 (R) - 甘醇和9种衍生物时,获得了高的反选择性.
- 证明了从碳酸到醇的单合成.
结论:
- 开发的P450系统提供了一种安全高效的方法来制造性糖醇.
- 这种方法最大限度地减少了H2O2的积累,防止了潜在的毒性.
- 该策略适用于合成各种醇衍生物.
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