Bioinspired Dual-Enzyme Colloidosome Reactors for High-Performance Biphasic Catalysis

Abstract

In this paper, a novel method for the construction of colloidosomes as a microreactor for dual-enzyme cascade biphasic reaction has been reported. A lipase–glucose oxidase (GOx) enzyme pair is employed in this system. A water-soluble enzyme GOx is compartmentalized inside the colloidosomes. A hydrophobic environment-favored enzyme Candida Antarctica lipase B (CalB) is adsorbed on the outer surfaces of the colloidosomes. The catalysis system is set up by introducing these dual-enzyme-immobilized microcapsules into acetic ether. H2O2 is produced in the aqueous phase by the doped GOx, and then H2O2 diffused out of the microcapsules is utilized by CalB to catalyze the oxidation of ethyl acetate. Finally, the formed peracids oxidized N-heteroaromatic in situ. Furthermore, no obvious yield decline is observed in four reaction cycles. Thus, our work provides a new strategy for the design of high-performance biomimicking reactors for multiple enzyme cascade reactions and further expands the potential application area of colloidosomes.

Immobilization of Multi-Enzymes on Support Materials for Efficient Biocatalysis

“…A ultrathin, hybrid silica microcapsule was designed to construct an efficient multi-enzyme system for the production of methanol from CO 2 (Wang et al, 2014), which was prepared through the deposition of catechol-modified gelatin, followed by in situ growth of silica nanoparticles on the gelatin layer. Formate dehydrogenase (FateDH), formaldehyde dehydrogenase (FaldDH), and alcohol dehydrogenase (YADH) were immobilized through physical entrapment in the microcapsule FIGURE 8 | Schematic illustration of the fabrication of the dual-enzyme colloidosome reactor for biphasic catalysis of pyridine (MTBE is tert-butyl methyl ether and TMOS is tetramethyl orthosilicate) (Liu et al, 2018). Reproduced with permission from ACS publications.…”

“…Moreover, a poly(acrylic acid) brushes-nanospherical silica was also used as co-immobilized support for the construction of a bienzymatic biosensor for glucose detection (Zhao et al, 2016). A colloidosome composed of SiO 2 nanoparticles was synthesized as the microreactor for dualenzyme cascade biphasic reaction (Figure 8), in which GOx was compartmentalized inside the colloidosome and Candida antarctica lipase (CalB) was adsorbed on the outer surfaces of the colloidosome (Liu et al, 2018). Glucose, as the energy source, was catalyzed by GOx to produce hydrogen peroxide (H 2 O 2 ) and H 2 O 2 diffused out of the microcapsules was employed by CalB to catalyze the perhydrolysis of ethyl acetate.…”

“… Schematic illustration of the fabrication of the dual-enzyme colloidosome reactor for biphasic catalysis of pyridine (MTBE is tert -butyl methyl ether and TMOS is tetramethyl orthosilicate) (Liu et al, 2018 ). Reproduced with permission from ACS publications.…”

Interface Engineering in Multiphase Systems toward Synthetic Cells and Organelles: From Soft Matter Fundamentals to Biomedical Applications

“…[146,148] Although nanoparticle layer is not as similar to cellular membranes as lipid bilayer, they can be explored to investigate cell-like behavior, and used as microreactors, delivery vehicles. [50,[149][150][151][152][153][154][155]…”

“…The most demonstrated and utilized enzymatic cascade is the glucose oxidase (GOx) and horseradish peroxidase (HRP) cascade, in which GOx oxidizes glucose to produce H 2 O 2 , a oxidizing substrate for HRP. [39,131,150,233,247,259,[328][329][330][331][332][333][334][335] The GOx-HRP cascades can also be performed in coacervate droplets as membraneless organelles, by cationizing or anionizing GOx and HRP respectively (Figure 16a). [233,247,253,259,270,333,334,336,337] A complicated version of the glucose cascade is presented in a synthetic beta cell, a multicompartmental vesosomes composed of an outer vesicle with glucose transporter 2 (GLUT2) and inner pH-responsive vesicles containing insulin (Figure 16b).…”