Highly Enantioselective Catalysis by Enzyme Encapsulated in Metal Azolate Frameworks with Micelle-Controlled Pore Sizes,ACS Central Science

当前位置： X-MOL 学术 › ACS Cent. Sci. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Highly Enantioselective Catalysis by Enzyme Encapsulated in Metal Azolate Frameworks with Micelle-Controlled Pore Sizes
ACS Central Science ( IF 12.7 ) Pub Date : 2024-01-18 , DOI: 10.1021/acscentsci.3c01432
Hao Ren ₁ , Jian Yuan ₂ , Yi-Ming Li _{1,

3} , Wen-Jing Li ₁ , Yi-Hang Guo _{4,

5} , Yi-Bo Zhang ₅ , Bing-Hao Wang ₁ , Kaili Ma ₆ , Lu Peng ₆ , Guping Hu ₇ , Wen-Qi Wang ₈ , Hailong He ₈ , Lien-Yang Chou ₈ , Ming-Hua Zeng ₅ , Yue-Biao Zhang ₈ , Lin Cheng ₁

Affiliation

Encapsulating enzymes within metal–organic frameworks has enhanced their structural stability and interface tunability for catalysis. However, the small apertures of the frameworks restrict their effectiveness to small organic molecules. Herein, we present a green strategy directed by visible linker micelles for the aqueous synthesis of MAF-6 that enables enzymes for the catalytic asymmetric synthesis of chiral molecules. Due to the large pore aperture (7.6 Å), double the aperture size of benchmark ZIF-8 (3.4 Å), MAF-6 allows encapsulated enzyme BCL to access larger substrates and do so faster. Through the optimization of surfactants’ effect during synthesis, BCL@MAF-6-SDS (SDS = sodium dodecyl sulfate) displayed a catalytic efficiency (K_cat/K_m) that was 420 times greater than that of BCL@ZIF-8. This biocomposite efficiently catalyzed the synthesis of drug precursor molecules with 94–99% enantioselectivity and nearly quantitative yields. These findings represent a deeper understanding of de novo synthetic encapsulation of enzyme in MOFs, thereby unfolding the great potential of enzyme@MAF catalysts for asymmetric synthesis of organics and pharmaceuticals.

中文翻译：

封装在具有胶束控制孔径的金属氮唑盐框架中的酶的高度对映选择性催化

将酶封装在金属有机框架内增强了其结构稳定性和催化界面的可调性。然而，框架的小孔径限制了它们对小有机分子的有效性。在此，我们提出了一种由可见连接胶束指导的用于 MAF-6 水合成的绿色策略，该策略使酶能够催化手性分子的不对称合成。由于孔径较大 (7.6 Å)，是基准 ZIF-8 (3.4 Å) 孔径尺寸的两倍，MAF-6 允许封装的酶 BCL 接触更大的底物，并且速度更快。通过优化合成过程中表面活性剂的作用，BCL@MAF-6-SDS（SDS=十二烷基硫酸钠）的催化效率（ K _cat / K _m ）是BCL@ZIF-8的420倍。这种生物复合材料有效地催化了药物前体分子的合成，具有 94-99% 的对映选择性和接近定量的产率。这些发现代表了对MOF中酶的从头合成封装的更深入的了解，从而展现了酶@MAF催化剂在有机物和药物不对称合成中的巨大潜力。

更新日期：2024-01-18

点击分享查看原文

点击收藏

公开下载

阅读更多本刊新发论文本刊介绍/投稿指南