Enhanced Catalysis via Multiscale Force Propagation in All-Enzyme Glucose Oxidase Hydrogels
Year: 2026
Type: preprint
Abstract: Enzyme-based biomaterials are sustainable catalytic platforms with applications in biosensing, pharmaceutical synthesis, and environmental remediation. A key challenge is developing universal immobilisation strategies that preserve activity without requiring enzyme-specific optimisation. One promising approach is the photochemical cross-linking of native tyrosine residues to form self-supporting all-enzyme hydrogels, where the enzyme serves as both the catalytic and structural component. However, rational design of these materials requires understanding how gelation-induced forces propagate through the network and influence enzyme function. Here, we combine experiments and simulations to establish a multiscale framework linking hydrogel assembly, force propagation, and catalysis in glucose oxidase hydrogels. By varying the lamp intensity used during photochemical cross-linking, we control gelation kinetics and examine their consequences across molecular and network length scales. Slower gelation reduces enzyme unfolding and produces more loosely packed hydrogel networks with enhanced dynamic correlations and increased free volume around enzyme active sites. Integrating experimental measurements with modelling reveals that these structural changes enhance catalytic performance through altered force transmission across the network. Our findings demonstrate that enzyme activity is regulated not only by local active-site processes but also by collective mechanical interactions spanning multiple length scales, establishing network mechanics as a new design principle for functional biocatalytic materials.
Source: ChemRxiv
Language: English
Subfield: Biomaterials
Field: Materials Science
Domain: Physical Sciences
Open Access status: green
Awards: G1689194922, G3537589354, G6271517897, IMR-MIP DANSE - Distributed Data Analysis for Neutron Scattering Experiments - CNST, MESONET: Exploiting in situ protein unfolding to understand and control mesoscopic network formation, G8681885083, Exploiting Engineered Polyproteins in the Modular Design of Robust, Tuneable and Biofunctional Hydrogels
OpenAlex ID: W7215083918