WP1 will construct structural 3D models, simulate the catalytic reactions, provide detailed analysis of the observed thermodynamic activation parameters (ΔG‡, ΔH‡ and ΔS‡) and suggest mutations for experimental investigation in WP4. Here the empirical valence bond (EVB) method will be utilised beneficially. EVB relies on parameterization of a suitable reference reaction, either ab initio surfaces or experimental rate constants, to reproduce the activation barrier and reaction free energy. Once this has been obtained, three distinct stages are required. Stage 1 involves the process of building and parameterizing the molecular system, calibration of EVB Hamiltonian to get the activation free energy, Stage 2 repeats the simulations at different temperatures to get the entalpic and entropic contributions, and Stage 3 analysis of the simulations and simulations of suggested mutations. Mutations predicted to affect the enthalpy-entropy balance will then be passed on to WP4 for experimental testing.
