Mechanistic Insight into Switching between H2- or O2-Activation by Simple Ligand Effects of [NiFe]hydrogenase Models

Takahiro Matsumoto; Takahiro Kishima; Takeshi Yatabe; Ki Seok Yoon; Seiji Ogo

doi:10.1021/acs.organomet.7b00471

Mechanistic Insight into Switching between H₂- or O₂-Activation by Simple Ligand Effects of [NiFe]hydrogenase Models

Takahiro Matsumoto, Takahiro Kishima, Takeshi Yatabe, Ki Seok Yoon, Seiji Ogo

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

7 Citations (Scopus)

Abstract

We present a mechanistic investigation for the activation of H₂ and O₂, induced by a simple ligand effect within [NiFe] models for O₂-tolerant [NiFe]hydrogenase. Kinetic study reveals Michaelis-Menten type saturation behaviors for both H₂ and O₂ activation, which is the same behavior as that found in O₂-tolerant [NiFe]hydrogenase. Such saturation behavior is caused by H₂ complexation followed by heterolytic cleavage of H₂ by an outer-sphere base, resulting in the formation of a hydride species showing hydridic character.

Original language	English
Pages (from-to)	3883-3890
Number of pages	8
Journal	Organometallics
Volume	36
Issue number	20
DOIs	https://doi.org/10.1021/acs.organomet.7b00471
Publication status	Published - Oct 23 2017

All Science Journal Classification (ASJC) codes

Physical and Theoretical Chemistry
Organic Chemistry
Inorganic Chemistry

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title = "Mechanistic Insight into Switching between H2- or O2-Activation by Simple Ligand Effects of [NiFe]hydrogenase Models",

abstract = "We present a mechanistic investigation for the activation of H2 and O2, induced by a simple ligand effect within [NiFe] models for O2-tolerant [NiFe]hydrogenase. Kinetic study reveals Michaelis-Menten type saturation behaviors for both H2 and O2 activation, which is the same behavior as that found in O2-tolerant [NiFe]hydrogenase. Such saturation behavior is caused by H2 complexation followed by heterolytic cleavage of H2 by an outer-sphere base, resulting in the formation of a hydride species showing hydridic character.",

author = "Takahiro Matsumoto and Takahiro Kishima and Takeshi Yatabe and Yoon, {Ki Seok} and Seiji Ogo",

note = "Funding Information: This work was supported by Grants-in-Aid: JP26000008 (Specially Promoted Research), JP16K05727, and JP15K05566 from Japan Society for the Promotion of Science (JSPS), and the World Premier International Research Centre Initiative (WPI), Japan. Publisher Copyright: {\textcopyright} 2017 American Chemical Society.",

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doi = "10.1021/acs.organomet.7b00471",

language = "English",

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AU - Matsumoto, Takahiro

AU - Kishima, Takahiro

AU - Yatabe, Takeshi

AU - Yoon, Ki Seok

AU - Ogo, Seiji

N1 - Funding Information: This work was supported by Grants-in-Aid: JP26000008 (Specially Promoted Research), JP16K05727, and JP15K05566 from Japan Society for the Promotion of Science (JSPS), and the World Premier International Research Centre Initiative (WPI), Japan. Publisher Copyright: © 2017 American Chemical Society.

PY - 2017/10/23

Y1 - 2017/10/23

N2 - We present a mechanistic investigation for the activation of H2 and O2, induced by a simple ligand effect within [NiFe] models for O2-tolerant [NiFe]hydrogenase. Kinetic study reveals Michaelis-Menten type saturation behaviors for both H2 and O2 activation, which is the same behavior as that found in O2-tolerant [NiFe]hydrogenase. Such saturation behavior is caused by H2 complexation followed by heterolytic cleavage of H2 by an outer-sphere base, resulting in the formation of a hydride species showing hydridic character.

AB - We present a mechanistic investigation for the activation of H2 and O2, induced by a simple ligand effect within [NiFe] models for O2-tolerant [NiFe]hydrogenase. Kinetic study reveals Michaelis-Menten type saturation behaviors for both H2 and O2 activation, which is the same behavior as that found in O2-tolerant [NiFe]hydrogenase. Such saturation behavior is caused by H2 complexation followed by heterolytic cleavage of H2 by an outer-sphere base, resulting in the formation of a hydride species showing hydridic character.

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Mechanistic Insight into Switching between H₂- or O₂-Activation by Simple Ligand Effects of [NiFe]hydrogenase Models

Abstract

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