Journal
JOURNAL OF PHYSICS-CONDENSED MATTER
Volume 29, Issue 36, Pages -Publisher
IOP PUBLISHING LTD
DOI: 10.1088/1361-648X/aa7db6
Keywords
oxygen reduction reaction; Au(111) surface; density functional theory calculations
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Funding
- National Natural Science Foundation of China [21576008, 91634116, 91334203, 21476020]
- Fundamental Research Funds for the Central Universities [PYCC1705]
- PetroChina Innovation Foundation [2016D-5007-0505]
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Oxygen reduction and hydrogen peroxide reduction are technologically important reactions in energy-conversion devices. In this work, a full understanding of oxygen reduction reaction (ORR) mechanism on Au(1 1 1) surface is investigated by density functional theory (DFT) calculations, including the reaction mechanisms of O-2 dissociation, OOH dissociation, and H2O2 dissociation. Among these ORR mechanisms on Au(1 1 1), the activation energy of O-2* hydrogenation reaction is much lower than that of O-2* dissociation, indicating that O-2* hydrogenation reaction is more appropriate at the first step than O-2* 2 dissociation. In the following, H2O2 can be formed with the lower activation energy compared with the OOH dissociation reaction, and finally H2O2 could be generated as a detectable product due to the high activation energy of H2O2 dissociation reaction. Furthermore, the potential dependent free energy study suggests that the H2O2 formation is thermodynamically favorable up to 0.4 V on Au(1 1 1), reducing the overpotential for 2e(-) ORR process. And the elementary step of first H2O formation becomes non-spontaneous at 0.4 V, indicating the difficulty of 4e(-) reduction pathway. Our DFT calculations show that H2O2 can be generated on Au(1 1 1) and the first electron transfer is the rate determining step. Our results show that gold surface could be used as a good catalyst for small-scale manufacture and on-site production of H2O2.
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