Electrochemical Atomic Force Microscopy and First-Principles Calculations of Ferriprotoporphyrin Adsorption and Polymerization

Langmuir : the ACS Journal of Surfaces and Colloids
Jason A BennettEva Zurek

Abstract

The adsorption and subsequent electrooxidative polymerization of ferriprotoporphyrin IX chloride (hemin; FePPCl) was investigated on highly ordered pyrolytic graphite, glassy carbon, and polycrystalline Pt electrodes using electrochemical atomic force microscopy, first-principles calculations, and cyclic voltammetry. Hemin was shown to readily adsorb to all three surfaces; however, it was more continuous over the carbon surfaces compared to the Pt surface. This disparity in adsorption appears to be a major contributing factor to differences observed between the electrodes following hemin electropolymerization. Despite differences in roughness and morphology, hemin polymerized as a continuous layer over each electrode surface. Periodic density functional theory calculations were used to model FePP (without Cl) on both the Pt(111) and graphite surfaces using the vdW-DF-optPBE functional to account for the dispersion interactions. Our calculations suggest that the FePP molecule chemisorbs to the Pt surface while at the same time exhibiting intramolecular hydrogen bonding between the carboxylic acid groups, which are extended away from the surface. In contrast to FePP-Pt chemisorption, FePP was found to physisorb to graphite. The p...Continue Reading

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