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Ash, J. E.

Publications and source records attributed to Ash, J. E..

2 recordsLinked to original sources

Graph attention with structural features improves the generalizability of identifying functional sequences at a protein interface

Accurate prediction of the set of sequences compatible with a protein-protein interface is an unsolved problem in biology. While supervised sequence-based models trained directly on experimental data can predict variant effects, they often fail to generalize to significantly diverged sequences. We hypothesized that incorporating information from deep learning models of proteins (e.g., ESM, ProteinMPNN) could enhance generalizability. To test this hypothesis, we designed and experimentally screened several deep mutational libraries of the SARS-CoV-2 Spike Receptor Binding Domain (RBD) for binding to the ACE2 receptor. Our large dataset encompasses over 43,000 sequence variants, exhibiting up to 26 substitutions away from the parental RBD sequence, thus exploring a significantly expanded sequence space compared to previous studies. Baseline supervised learning with one-hot encoded sequences achieved high accuracy within training sets but poor performance on unseen libraries. Integrating pre-trained protein model embeddings (ESM2) as a feature showed modest improvement in generalization. To further enhance predictive power, we developed a graph attention network architecture that combines representations of local residue environments using protein structure graphs with long-range inter-residue correlations captured by protein language model (PLM) embeddings (GAN-PLM). By explicitly modeling residue environments, interface geometry, and sequence dependencies, our graph attention model outperformed purely sequence-based models, achieving substantially higher balanced accuracies when predicting functional ACE2-binding variants across the diverse sequence space spanned by our independent libraries. This demonstrates the potential of structure- and sequence-based features into deep learning frameworks to achieve accurate and generalizable predictions of protein interface function, with broad implications for understanding and engineering protein interactions relevant to emerging infectious diseases and therapeutic protein design.

biochemistry↗

Acoustic Force Spectroscopy Reveals Subtle Differences in Cellulose Unbinding Behavior of Carbohydrate-Binding Modules

To rationally engineer more efficient cellulolytic enzymes for cellulosic biomass deconstruction into sugars for biofuels production, it is necessary to better understand the complex enzyme-substrate interfacial interactions. Carbohydrate binding modules (CBM) are often associated with microbial surface-tethered cellulosomal or freely secreted cellulase enzymes to increase substrate accessibility. However, it is not well known how CBM recognize, bind, and dissociate from polysaccharide surfaces to facilitate efficient cellulolytic activity due to the lack of mechanistic understanding of CBM-substrate interactions. Our work outlines a general approach to methodically study the unbinding behavior of CBMs from model polysaccharide surfaces using single-molecule force spectroscopy. Here, we apply acoustic force spectroscopy (AFS) to probe a Clostridium thermocellum cellulosomal scaffoldin protein (CBM3a) and measure its dissociation from nanocellulose surfaces at physiologically relevant, low force loading rates. An automated microfluidic setup and methodology for uniform deposition of insoluble polysaccharides on the AFS chip surfaces is demonstrated. The rupture forces of wild-type CBM3a, and its Y67A mutant, unbinding from nanocellulose surface suggests distinct CBM binding conformations that can also explain the improved cellulolytic activity of cellulase tethered to CBM. Applying established dynamic force spectroscopy theory, the single-molecule unbinding rate at zero force is extrapolated and found to agree well with bulk equilibrium unbinding rates estimated independently using quartz crystal microbalance with dissipation monitoring. However, our results highlight the limitations of applying classical theory to explain the highly multivalent CBM-cellulose interactions seen at higher cellulose-CBM bond rupture forces (>15pN). Significance StatementCellulases are multi-modular enzymes produced by numerous microbes that catalyze cellulose hydrolysis into glucose. These enzymes play an important role in global carbon cycling as well as cellulosic biofuels production. CBMs are essential components of cellulolytic enzymes involved in facilitating hydrolysis of polysaccharides by tethered catalytic domains (CD). The subtle interplay between CBM binding and CD activity is poorly understood particularly for heterogeneous reactions at solid-liquid interfaces. Here, we report a highly multiplexed single-molecule force spectroscopy method to study CBM dissociation from cellulose to infer the molecular mechanism governing substrate recognition and dissociation. This approach can be broadly applied to study multivalent protein-polysaccharide binding interactions relevant to other carbohydrates such as starch, chitin, or hyaluronan to engineer efficient biocatalysts.

biochemistry↗