화학공학소재연구정보센터
International Journal of Hydrogen Energy, Vol.42, No.4, 2278-2287, 2017
Exploring metal decorated Porphyrin-like Porous Fullerene as catalyst for oxygen reduction reaction: A DFT study
The development of highly active and non-precious catalyst for the oxygen reduction reaction (ORR) at the cathode has been a key challenge for the commercial application of fuel cells in large scale. In this work, we have explored new kind of non-precious catalyst, viz. transition metal decorated porous carbon nitride fullerene (M-C24N24, M = Fe, Co, and Ni) for ORR by using density functional theory as a tool. It was found that these metal atoms, decorated on Porphyrin-like Porous Fullerene, did not tend to aggregate. We have systematically investigated the feasibility of ORR reaction on Fe, Co and Ni-decorated C24N24 systems. To get a primary knowledge about the activity, we have compared the oxygen adsorption energy on these three systems. Then we have calculated the free energies for the intermediate steps to demonstrate the preferred path of oxygen reduction reaction. Interestingly, oxygen reduction reaction is found to proceed through the more efficient four electron reduction path. More interestingly, all the reaction steps are found to be spontaneous on both Fe-C24N24 and Co-C24N24. To draw final conclusion regarding the most efficient catalyst among the three systems, we also analyze the free energy profiles at different electrode potentials. (C) 2016 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.