What Bob Parr has wrought: Quantum mechanics based reaction mechanisms for electrocatalysis

Abstract

Bob Parr, along with major contributions by Levy and Perdew, provided the key advances in understanding the foundation of D. Function Theory that underlies the major advances in theory and computation in predicting the mechanisms of complex electrocatalytic reactions, which is now leading to new in silica design that is being validated exptl. We will highlight some recent advances in such methodologies including: Grand canonical QM calcns. of electrochem. catalysis at canst. potential (instead of canst. nos. of electrons), QM Metadynamics calcns. of free energies of electrocatalysis at operational temp. and potential which we will illustrate with recent applications to catalytic systems including: The reaction mechanism for the Electrocatalytic oxygen redn. reaction on Pt(111) and Pt alloys. Crit. potentials and reaction mechanisms for CO2 redn. to form hydrocarbon fuels on (100) and (111) Cu surfaces at various pH (0 to 14), Acceleration of CO2 redn. on nanoparticles. The MEOM mixed oxide-metal mechanism for accelerated CO2 redn. The reaction mechanism for the Electrocatalytic oxygen evolution on Fe doped NiOOH.