Zhang Ming, Wang Minran, Mi Yumeng, Li Ting, Hou Dawei, Li Haitao, Tong Xili, Zhang Tingting, Yi Huimin, Yang Hengquan
Engineering Research Center of Ministry of Education for Fine Chemicals, Shanxi Key Laboratory of Coal-based Value-added Chemicals Green Catalysis Synthesis, School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan, China.
Shanxi Research Institute of Huairou Laboratory, Taiyuan, China.
Nat Commun. 2025 Aug 29;16(1):8087. doi: 10.1038/s41467-025-63476-1.
The practical applications of enzymes often require their immobilization for multiple recycling or long-term running. However, practically efficient enzyme immobilization methods are lacking. Herein, we present an enzyme immobilization approach by engineering a porous "interphase" between water and oil around the surfaces of Pickering emulsion droplets. The designed "interphase" consists of a porous, nanometer-thick silica shell serving as a scaffold to incorporate enzymes. Within this "interphase", enzymes can simultaneously be in contact with enzyme-preferred aqueous microenvironment and the oil phase containing organic reactants. The porous "interphase" with its tunable structure and properties allows modulation of transport of reactants, crudely akin to a cell membrane, and of local concentration of reactants. As a proof of the concept, we showcase that our "interphase" strategy is very effective in immobilization of Candida antarctica lipase B (CALB) for continuous-flow olefin epoxidation. Long-term stabilization (800 h), 16-fold increase in catalysis efficiency relative to batch reactions, and 99% HO utilization efficiency are achieved. The integration of unique microenvironment and hydrophobic pores of the "interphase" is found to be crucial for such excellent performances, practically providing the most efficient enzymatic epoxidation system. This strategy opens an avenue for the design of efficient and sustainable biocatalytic processes.
酶的实际应用通常需要将其固定化以实现多次循环利用或长期运行。然而，目前缺乏实用高效的酶固定化方法。在此，我们提出一种酶固定化方法，通过在皮克林乳液液滴表面构建水与油之间的多孔“界面相”。所设计的“界面相”由多孔的纳米厚二氧化硅壳组成，作为容纳酶的支架。在这个“界面相”内，酶可以同时与酶偏好的水性微环境以及含有有机反应物的油相接触。具有可调结构和性质的多孔“界面相”能够调节反应物的传输，大致类似于细胞膜，以及反应物的局部浓度。作为概念验证，我们展示了我们的“界面相”策略在固定南极假丝酵母脂肪酶B（CALB）用于连续流烯烃环氧化方面非常有效。实现了长期稳定性（800小时），相对于间歇反应催化效率提高了16倍，以及99%的过氧化氢利用效率。发现“界面相”独特的微环境和疏水孔的整合对于如此优异的性能至关重要，实际上提供了最有效的酶促环氧化系统。该策略为设计高效且可持续的生物催化过程开辟了一条途径。
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