Sun Zhiyong, Glebe Ulrich, Charan Himanshu, Böker Alexander, Wu Changzhu
Institute of Microbiology, Technische Universität Dresden, Zellescher Weg 20b, 01217, Dresden, Germany.
Fraunhofer Institute for Applied Polymer Research IAP, Geiselbergstrasse 69, 14476, Potsdam-Golm, Germany.
Angew Chem Int Ed Engl. 2018 Oct 15;57(42):13810-13814. doi: 10.1002/anie.201806049. Epub 2018 Sep 21.
Despite the rapid development of Pickering interfacial catalysis (PIC) at liquid-liquid interfaces with chemocatalysts, the use of unstable biocatalysts at emulsion interfaces remains a technical challenge. Herein, we present a Pickering interfacial biocatalysis (PIB) platform based on robust and recyclable enzyme-polymer conjugates that act as both catalytic sites and stabilizers at the interface of Pickering emulsions. The conjugates were prepared by growing poly(N-isopropylacrylamide) on a fragile enzyme, benzaldehyde lyase, under physiological conditions. The mild in situ conjugation process preserved the enzyme structure, and the conjugates were used to emulsify a water-organic two-phase system into a stable Pickering emulsion, leading to a significantly larger interfacial area and a 270-fold improvement in catalytic performance as compared to the unemulsified two-phase system. The PIB system could be reused multiple times. Conjugates of other enzymes were also fabricated and applied for cascade reactions.
尽管在液-液界面使用化学催化剂的皮克林界面催化（PIC）发展迅速，但在乳液界面使用不稳定的生物催化剂仍然是一项技术挑战。在此，我们提出了一种基于坚固且可回收的酶-聚合物共轭物的皮克林界面生物催化（PIB）平台，该共轭物在皮克林乳液界面既作为催化位点又作为稳定剂。共轭物是通过在生理条件下在脆弱的酶苯甲醛裂解酶上生长聚（N-异丙基丙烯酰胺）制备的。温和的原位共轭过程保留了酶的结构，并且共轭物用于将水-有机两相体系乳化形成稳定的皮克林乳液，与未乳化的两相体系相比，导致界面面积显著增大且催化性能提高了270倍。PIB系统可以重复使用多次。还制备了其他酶的共轭物并将其应用于级联反应。
