THE MECHANISM OF THE OXYGEN REDUCTION REACTION FROM DFT CALCULATIONS; IMPLICATIONS FOR IMPROVED CATALYSTS

摘要

Proton Exchange Membrane fuel cells (PEMFC) are most promising emission free energy systems for homes and families. However, the kinetics for the catalytic oxygen reduction reaction (ORR) 1/2 O2 + 2 H~+ + 2 e -> H2O remain too slow, increasing the amount and cost of the catalyst to too high a level for widespread application. To use Density Functional Theory (DFT) to determine how the barrier would change for new alloys, a critical issue is to account for the dependence of the electron transfer steps on the external electrochemical potential. To accomplishe this we developed a systematic approach for handling the electron transfer step along with the solvation effects and including the effect of the external electrochemical potential on the electron transfer reactions involved in ORR.