High Adsorption of α-Glucosidase on Polymer Brush-Modified Anisotropic Particles Acquired by Electrospraying—A Combined Experimental and Simulation Study

Abstract

In this particular contribution, we aim to immobilize a model enzyme such as α-glucosidase onto poly(DMAEMA) [poly(2-dimethyl amino ethyl methacrylate)] brush-modified anisotropic (cup-and disc-shaped) biocompatible polymeric particles. The anisotropic particles comprising a blend of PLA [poly(lactide)] and poly(MMA-co-BEMA) [poly((methyl methacrylate)-co-(2-(2-bromopropionyloxy) ethyl methacrylate)] were acquired by electrospraying, a scalable and convenient technique. We have also demonstrated the role of a swollen polymer brush grafted on the surface of cup-/disc-shaped particles via surfaceinitiated atom transfer radical polymerization in immobilizing an unprecedentedly high loading of enzyme [441 mg/g (cup)−589 mg/g (disc) of particles, 15−20 times higher than that of the literature-reported system] as compared to non-brush-modified particles. Circular dichroism spectroscopy was used to predict the structural changes of the enzyme upon immobilization onto the carrier particles. An enormously high amount of enzymes with preserved activity (∼85 ± 13% for cups and ∼78 ± 15% for discs) was found to adhere onto brush-modified particles at pH 7 via electrostatic adsorption. These findings were further explored at the atomistic level using a coarse-grained dissipative particle dynamics simulation approach, which exhibited excellent correlation with experimental results. In addition, accelerated particle separation was also achieved via magnetic force-induced aggregation within 20 min (without a centrifuge) by incorporating magnetic nanoparticles into disc-shaped particles while electrojetting. This further strengthens the technical feasibility of the process, which holds immense potential to be applied for various enzymes intended for several applications.

Dissipative particle dynamics simulation study on ATRP-brush modification of variably shaped surfaces and biopolymer adsorption

“…14,15 Therefore, a controlled surface modification of the particles could be crucial to several biomedical applications. [16][17][18][19][20] There are numerous reports demonstrating the importance of surface modification of MPs such as polymeric cup-shaped particles using various techniques such as solvent evaporation, 13 vapor deposition, 21 mini-emulsion, 22,23 and microfluidics. 24 Among the numerous applications of surface-modified particles, the immobilization of biopolymers (e.g., enzymes) has been getting enormous attention in the last decade due to its use in biocatalysts, food processing, drug delivery, textile manufacturing, biosensors, and so on.…”

“…[25][26][27] This inspired researchers to find a better solution to utilize biopolymers more efficiently to expand their applications. 19,[28][29][30][31] Further, the immobilization of biopolymers on insoluble solid particles has enhanced the rapid arrest and controlled quenching of reaction kinetics. This is because of a comparatively more straightforward extraction of solid surface-bound biopolymers from the solution.…”

“…This is because of a comparatively more straightforward extraction of solid surface-bound biopolymers from the solution. 19,[28][29][30][31][32][33][34][35][36] Thus, this immobilization process improves the stability and reusability of biopolymers against the change in pH, solvent, and temperature over successive chemical reactions. [37][38][39] The immobilization of biopolymers on solid surfaces has significant medical and industrial applications.…”

“…38,39 Ifra and co-workers have recently illustrated differently shaped MP modifications using the electrojetting technique. [17][18][19] In particular, different MPs are prepared from a blend of polylactide (PLA) and poly[methylmethacrylate-co-2-(2-bromopropionyloxy)ethyl methacrylate] (poly(MMA-co-BEMA)) in 3 : 1 ratio. 17 To fabricate the surface, poly(DMAEMA) brushes are synthesized via the grafting from approach at the initiator (BEMA molecule) embedded surfaces via atom transfer radical polymerization (ATRP) [17][18][19] with DMAEMA monomers in water (pH B 7).…”

“…[17][18][19] In particular, different MPs are prepared from a blend of polylactide (PLA) and poly[methylmethacrylate-co-2-(2-bromopropionyloxy)ethyl methacrylate] (poly(MMA-co-BEMA)) in 3 : 1 ratio. 17 To fabricate the surface, poly(DMAEMA) brushes are synthesized via the grafting from approach at the initiator (BEMA molecule) embedded surfaces via atom transfer radical polymerization (ATRP) [17][18][19] with DMAEMA monomers in water (pH B 7). The brush grafting density is regulated by altering the initiator concentration on the surfaces.…”