Abstract
Oxygen tolerance capacity is critical for hydrogen oxidation/evolution catalysts. In nature, [NiFe] hydrogenases show excellent O2-tolerance and can rapidly reactivate the active site. This work aims to understand the reduction of O2 on the active site of [NiFe] hydrogenases. From the density functional theory (DFT) calculations, the free energy diagram for the oxygen reduction reaction (ORR) has been derived and the rate-determining step is found to be the Ni-B to Ni-SIb′ step. Our calculation explains the slow reactivation for the Ni-A state compared to the Ni-B state, which is due to the particularly stable structure of the Ni-A state.
Original language | English |
---|---|
Pages (from-to) | 23528-23534 |
Number of pages | 7 |
Journal | Physical Chemistry Chemical Physics |
Volume | 20 |
Issue number | 36 |
DOIs | |
Publication status | Published - 24 Aug 2018 |