文献类型：期刊文献

英文题名：Hierarchical Porous Silica Aerogel Monoliths for High-Flow Rate Continuous-Flow Enzyme Catalysis

作者：Deng, Xuelei[1];Liu, Jiaxu[1];Zhang, Xiaoyan[1];Fan, Daidi[2];Zhang, Zichen[3];Bai, Yunpeng[1,2]

机构：[1]East China Univ Sci & Technol, Coll Biotechnol, Shanghai Collaborat Innovat Ctr Biomfg, State Key Lab Bioreactor Engn, Shanghai 200237, Peoples R China;[2]Northwest Univ, Shaanxi R&D Ctr Biomat & Fermentat Engn, Sch Chem Engn, Xian 710069, Shaanxi, Peoples R China;[3]Beihang Univ, Sch Integrated Circuit Sci & Engn, Natl Key Lab Spintron, Beijing 100191, Peoples R China

年份：2025

卷号：13

期号：16

起止页码：5852

外文期刊名：ACS SUSTAINABLE CHEMISTRY & ENGINEERING

收录：;EI(收录号：20251618257185);WOS:【SCI-EXPANDED(收录号:WOS:001467509700001)】；

基金：This work was financially sponsored by the National Natural Science Foundation of China (grant nos. 22378120 and 22078096).

语种：英文

外文关键词：enzyme immobilization; sol-gel; hierarchicallystructure; monoliths; continuous flow; carbonyl reductase; asymmetric reduction

摘要：The use of immobilized enzymes in the continuous-flow synthesis of fine chemicals enables the development of a sustainable chemical industry. However, biocatalysis with immobilized enzymes in packed bed reactors is limited by the trade-off between activity and stability, diffusion limitation, and pressure drop. Here, a hierarchical porous silica aerogel monolith (HPSAM) microreactor encapsulating two coupled oxidoreductases was designed and prepared by the sol-gel method combined with an ice templating and freeze-drying technology. The HPSAM has a uniform and open porous structure characterized by 10-20 mu m flow-through macropores, and the kinetic analysis of the immobilized enzyme indicates that the reaction is not diffusion limited. The HPSAM microreactor can be operated at flow rates up to 20 mL/min (1.06 x 10-3 m/s) for a single reactor. As exemplified by the synthesis of chiral lactones, 30 mM (R)-gamma-decactone (3c) was obtained in 13 s with 82% conversion and 99% ee, affording a high space-time yield (STY, 27,184 g L-1 day-1) that was 23 times higher than the maximum STY reported for batch reactions. The microreactor maintained consistent performance throughout 2 weeks of continuous operation, with the total turnover number (TTN) of SmCRV4 reaching 1.05 x 105 during this period. Five chiral lactones were successfully synthesized by using this approach via flow asymmetric reduction. The HPSAM microreactors stored at 4 and 25 degrees C maintained excellent catalytic performance for at least 4 weeks.