Intermediates in the catalytic cycle of methyl coenzyme M reductase: Isotope exchange is consistent with formation of a σ-Alkane-Nickel Complex

Silvan Scheller; Meike Goenrich; Stefan Mayr; Rudolf K. Thauer; Bernhard Jaun

doi:10.1002/anie.201003214

Intermediates in the catalytic cycle of methyl coenzyme M reductase: Isotope exchange is consistent with formation of a σ-Alkane-Nickel Complex

Silvan Scheller^*, Meike Goenrich, Stefan Mayr, Rudolf K. Thauer, Bernhard Jaun

^*Corresponding author for this work

Not published at Aalto University

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Abstract

The key nickel enzyme for methanogenesis (MCR) catalyzes the formation of CH₃D and CH₂D₂ in a deuterated medium. CH ₂D₂ is formed by an exchange of deuterium into the S-methyl group of the substrate. Deuterium is incorporated at both carbon atoms of the S-ethyl group of ethyl coenzyme M, and a ¹³C label is rapidly scrambled within the ethyl group (see scheme). Thus, at least one intermediate is formed and the isotope exchange pattern is consistent with formation of a σ-alkane-nickel complex.

Original language	English
Pages (from-to)	8112-8115
Number of pages	4
Journal	Angewandte Chemie
Volume	49
Issue number	44
DOIs	https://doi.org/10.1002/anie.201003214
Publication status	Published - 25 Oct 2010
MoE publication type	A1 Journal article-refereed

Keywords

σ-alkane ligands
C-H activation
Isotope exchange
Methyl coenzyme M reductase
Nickel enzymes

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title = "Intermediates in the catalytic cycle of methyl coenzyme M reductase: Isotope exchange is consistent with formation of a σ-Alkane-Nickel Complex",

abstract = "The key nickel enzyme for methanogenesis (MCR) catalyzes the formation of CH3D and CH2D2 in a deuterated medium. CH 2D2 is formed by an exchange of deuterium into the S-methyl group of the substrate. Deuterium is incorporated at both carbon atoms of the S-ethyl group of ethyl coenzyme M, and a 13C label is rapidly scrambled within the ethyl group (see scheme). Thus, at least one intermediate is formed and the isotope exchange pattern is consistent with formation of a σ-alkane-nickel complex.",

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AU - Goenrich, Meike

AU - Mayr, Stefan

AU - Thauer, Rudolf K.

AU - Jaun, Bernhard

PY - 2010/10/25

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N2 - The key nickel enzyme for methanogenesis (MCR) catalyzes the formation of CH3D and CH2D2 in a deuterated medium. CH 2D2 is formed by an exchange of deuterium into the S-methyl group of the substrate. Deuterium is incorporated at both carbon atoms of the S-ethyl group of ethyl coenzyme M, and a 13C label is rapidly scrambled within the ethyl group (see scheme). Thus, at least one intermediate is formed and the isotope exchange pattern is consistent with formation of a σ-alkane-nickel complex.

AB - The key nickel enzyme for methanogenesis (MCR) catalyzes the formation of CH3D and CH2D2 in a deuterated medium. CH 2D2 is formed by an exchange of deuterium into the S-methyl group of the substrate. Deuterium is incorporated at both carbon atoms of the S-ethyl group of ethyl coenzyme M, and a 13C label is rapidly scrambled within the ethyl group (see scheme). Thus, at least one intermediate is formed and the isotope exchange pattern is consistent with formation of a σ-alkane-nickel complex.

KW - σ-alkane ligands

KW - C-H activation

KW - Isotope exchange

KW - Methyl coenzyme M reductase

KW - Nickel enzymes

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Intermediates in the catalytic cycle of methyl coenzyme M reductase: Isotope exchange is consistent with formation of a σ-Alkane-Nickel Complex

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