DFT-Binding Metadynamics

Role of Vicinal H bonding Groups to Organic Acid Catalyzed Glucan Hydrolysis

In this work, we studied the effect of hydrogen bonding moieties of acid catalysts in glucan hydrolysis. Benzoic acid and its derivatives served as model catalysts to mimic the character of oxidized activated carbon which was found to have acidic groups. Our initial study of glucan interaction with the model catalysts found that the stability of the complex is directly related to the catalytic activity in experiments. We further analyze the potential energy surface of the reactions and found that protonated system closely modeled the experimental activation energy. This suggested cooperation with the previously dissolved proton and the catalyst. To

study dynamic effects as well as finite temperature effects, we utilized Density Functional Theory Binding Metadynamics. Metadynamics is a biased sampling technique which hastens the simulation of rare events such as proton transfer reactions. This elucidated that the neighboring h-bonding group orients a solvated proton to the active site facilitating cleavage