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Incorporation of Metals and Enzymes with Porous Imine Molecule Cages for Highly Efficient Semiheterogeneous Chemoenzymatic Catalysis
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-04-22 , DOI: 10.1021/acscatal.1c00587 Shiqi Gao 1 , Yunting Liu 1 , Lihui Wang 1, 2 , Zihan Wang 1 , Pengbo Liu 1 , Jing Gao 1 , Yanjun Jiang 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-04-22 , DOI: 10.1021/acscatal.1c00587 Shiqi Gao 1 , Yunting Liu 1 , Lihui Wang 1, 2 , Zihan Wang 1 , Pengbo Liu 1 , Jing Gao 1 , Yanjun Jiang 1
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Combining the advantages of homogeneous and heterogeneous catalysis is highly desired but remains a challenging goal. Herein, we fabricated a semiheterogeneous metal–enzyme-integrated catalyst using soluble porous imine molecule cages (IMCs), which could partially dissolve in organic solvents under heating conditions for catalytic tasks while precipitate completely at room temperature for catalyst recovery. The IMCs play three vital roles: (1) acting as a support and stabilizer for metal nanoparticles and enzymes, (2) partially solubilizing the heterogeneous catalyst in organic medium, and (3) creating hydrophobic and basic microenvironments for improved catalytic efficiency. The covalent immobilization of the enzyme by utilizing imine bonds via the Ugi-type reaction was disclosed, in which the effect of different parameters on enzyme immobilization and the structure–activity relationship were investigated. The semiheterogeneous catalyst exhibited high activity, selectivity, and reusability in chemoenzymatic dynamic kinetic resolution of amines at low temperature (50–60 °C) with high yields and enantioselectivities (up to 94% yield and 98% ee).
中文翻译：
金属和酶与多孔亚胺分子笼的结合，用于高效的半异构化学酶催化
高度希望结合均相和非均相催化的优点，但仍然是一个具有挑战性的目标。本文中，我们使用可溶性多孔亚胺分子笼（IMC）制备了半均相金属-酶集成催化剂，该笼可在加热条件下部分溶解于有机溶剂中以完成催化任务，而在室温下完全沉淀以回收催化剂。IMC发挥三个重要作用：（1）充当金属纳米颗粒和酶的载体和稳定剂；（2）将非均相催化剂部分溶解在有机介质中；（3）创建疏水性和碱性微环境以提高催化效率。公开了通过Ugi型反应利用亚胺键对酶进行共价固定，其中研究了不同参数对酶固定化的影响以及结构与活性之间的关系。这种半均相催化剂在低温（50–60°C）下具有高产率和对映选择性（高达94％的收率和98％的ee），在胺的化学酶动力学动力学拆分中显示出高活性，选择性和可重复使用性。
更新日期：2021-05-07
中文翻译：
金属和酶与多孔亚胺分子笼的结合，用于高效的半异构化学酶催化
高度希望结合均相和非均相催化的优点，但仍然是一个具有挑战性的目标。本文中，我们使用可溶性多孔亚胺分子笼（IMC）制备了半均相金属-酶集成催化剂，该笼可在加热条件下部分溶解于有机溶剂中以完成催化任务，而在室温下完全沉淀以回收催化剂。IMC发挥三个重要作用：（1）充当金属纳米颗粒和酶的载体和稳定剂；（2）将非均相催化剂部分溶解在有机介质中；（3）创建疏水性和碱性微环境以提高催化效率。公开了通过Ugi型反应利用亚胺键对酶进行共价固定，其中研究了不同参数对酶固定化的影响以及结构与活性之间的关系。这种半均相催化剂在低温（50–60°C）下具有高产率和对映选择性（高达94％的收率和98％的ee），在胺的化学酶动力学动力学拆分中显示出高活性，选择性和可重复使用性。
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