The oxygen reduction reaction on [NiFe] hydrogenases

Siyao Qiu; Seth Olsen; Douglas R. Macfarlane; Chenghua Sun

doi:10.1039/c8cp04160a

The oxygen reduction reaction on [NiFe] hydrogenases

Siyao Qiu, Seth Olsen, Douglas R. Macfarlane, Chenghua Sun

School of Chemistry

Research output: Contribution to journal › Article › Research › peer-review

4 Citations (Scopus)

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-SI_b′ 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	https://doi.org/10.1039/c8cp04160a
Publication status	Published - 24 Aug 2018

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10.1039/c8cp04160a

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Cite this

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title = "The oxygen reduction reaction on [NiFe] hydrogenases",

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.",

author = "Siyao Qiu and Seth Olsen and Macfarlane, {Douglas R.} and Chenghua Sun",

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doi = "10.1039/c8cp04160a",

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journal = "Physical Chemistry Chemical Physics",

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T1 - The oxygen reduction reaction on [NiFe] hydrogenases

AU - Qiu, Siyao

AU - Olsen, Seth

AU - Macfarlane, Douglas R.

AU - Sun, Chenghua

PY - 2018/8/24

Y1 - 2018/8/24

N2 - 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.

AB - 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.

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