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An investigation of possible competing mechanisms for Ni-containing methyl-coenzyme M reductase
Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.ORCID-id: 0000-0003-0702-7831
Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.ORCID-id: 0000-0001-7787-1881
Antal upphovsmän: 32014 (Engelska)Ingår i: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 16, nr 27, s. 14029-14035Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Ni-containing methyl-coenzyme M reductase (MCR) is capable of catalyzing methane formation from methyl-coenzyme M (CH3-SCoM) and coenzyme B (CoB-SH), and also its reverse reaction (methane oxidation). Based on extensive experimental and theoretical investigations, it has turned out that a mechanism including an organometallic methyl-Ni(III)F-430 intermediate is inaccessible, while another mechanism involving a methyl radical and a Ni(II)-SCoM species currently appears to be the most acceptable one for MCR. In the present paper, using hybrid density functional theory and an active-site model based on the X-ray crystal structure, two other mechanisms were studied and finally also ruled out. One of them, involving proton binding on the CH3-SCoM substrate, which should facilitate methyl-Ni(III)F-430 formation, is demonstrated to be quite unfavorable since the substrate has a much smaller proton affinity than the F-430 cofactor. Another one (oxidative addition mechanism) is also shown to be unfavorable for the MCR reaction, due to the large endothermicity for the formation of the ternary intermediate with side-on C-S (for CH3-SCoM) or C-H (for methane) coordination to Ni.

Ort, förlag, år, upplaga, sidor
2014. Vol. 16, nr 27, s. 14029-14035
Nationell ämneskategori
Kemi
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URN: urn:nbn:se:su:diva-106456DOI: 10.1039/c4cp01483aISI: 000338116700053OAI: oai:DiVA.org:su-106456DiVA, id: diva2:736126
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Tillgänglig från: 2014-08-05 Skapad: 2014-08-04 Senast uppdaterad: 2020-03-05Bibliografiskt granskad

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Blomberg, Margareta R. A.Siegbahn, Per E. M.
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Institutionen för organisk kemi
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Physical Chemistry, Chemical Physics - PCCP
Kemi

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