Biomimetic Cellulosomes Assembled on Molecular Brush Scaffolds: Random Complexes vs Enzyme Mixtures

• DOI: 10.1021/acsapm.0c01407
• Publication Date: 2021-03-16T23:50:36Z
• Authors: Oksana Zholobko; Ademola Hammed; Andrey Zakharchenko; Nikolay Borodinov; Igor Luzinov; Breeanna Urbanowicz; Taras Patsahan; Jaroslav Ilnytskyi; Sergiy Minko; Scott W. Pryor; Andriy Voronov
• Keywords: Carboxymethyl cellulose; Cellulosome

This work reports on the development of biomimetic polymeric cellulosomes—enzyme–polymer conjugates (EPCs) generated by covalent binding cellulase enzymes onto a molecular brush polymer scaffold synthesized radical copolymerization poly(ethylene glycol) methyl ether methacrylate (PEGMA) and glycidyl (GMA). In contrast to natural cellulosomes, EPC is in random process conjugation different cellulases from their mixture solution. The catalytic activity EPCs systematically studied using carboxymethyl cellulose, microcrystalline filter paper, pretreated switchgrass biomass substrates. exhibit improved with both soluble insoluble synergistic effect essential, multifold improvement substrate surface coverage enzyme being less than 50% saturation amount. Coarse-grained dynamics simulations provide evidence for increased concentration EPC-delivered motifs as compared number such randomly formed adsorption free enzymes, which good agreement experiments. increases diversity included structure also presence solutions. experiments reveal that reduce inhibitory depolymerization product (glucose), could facilitate higher hydrolysis rates at solid loadings. experimental results demonstrate arrangement complex, substantial comparable cellulosomes low enzyme-to-substrate ratio due combination complementary functions bound same close vicinity.