Bienzymatic Generation of Interpenetrating Polymer Networked Engineered Living Materials with Shape Changing Properties

Bienzymatic Generation of Interpenetrating Polymer Networked Engineered Living Materials with Shape Changing Properties
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DOI:
10.1002/admt.202300626
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发表时间:
2023-07
影响因子:
6.8
通讯作者:
R. Klemperer;Mark R. Shannon;J. L. Ross Anderson;A. Perriman
R. Klemperer;Mark R. Shannon;J. L. Ross Anderson;A. Perriman
中科院分区:
材料科学2区
文献类型:
--
作者:
R. Klemperer;Mark R. Shannon;J. L. Ross Anderson;A. Perriman

文献摘要

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描述了用于制造大规模(cm)可逆热敏结构的多孔形状变化互穿网络(IPN)生物链接的合成。采用辣根过氧化物酶(HRP)/葡萄糖氧化酶(GOx)双酶引发体系,在室温和有氧条件下,在离子交联海藻酸盐水凝胶中原位生成聚(N‐异丙基丙烯酰胺)(PNIPAm) IPN。IPN水凝胶的力学测试评估证实了通过共价单网互指的力学强化。此外,该热敏生物链接可用于打印含有基因工程磷酸三酯酶表达大肠杆菌的生物杂交反应器,这些大肠杆菌能够水解有毒的有机磷化合物。本文中,利用IPN的收缩-热敏响应来增加生物链接的孔径,提高了温度依赖的理论传质限制酶催化反应速率,为生物打印结构中外部调节的酶催化提供了可行的途径。
The synthesis of a porous shape‐changing interpenetrating network (IPN) bioink for the fabrication of large‐scale (cm) reversibly thermosensitive structures is described. The poly(N‐isopropylacrylamide) (PNIPAm) IPN is generated in situ within an ionically crosslinked alginate hydrogel at room temperature and under aerobic conditions using a horseradish peroxidase (HRP)/glucose oxidase (GOx) bienzymatic initiation system. Mechanical testing assessment of the IPN hydrogels confirm mechanical reinforcement via covalent single network interdigitation. Furthermore, the thermosensitive bioink can be used to print biohybrid reactors containing genetically engineered phosphotriesterase‐expressing E. coli capable of hydrolyzing toxic organophosphorus compounds. Herein, increasing the bioink pore size using the contractile‐thermosensitive response of the IPN improves the temperature‐dependent theoretical mass‐transfer‐limited enzyme catalyzed reaction rate, providing a plausible route to externally regulated enzymatic catalysis within bioprinted structures.