Document Type

Article

Language

eng

Format of Original

4 p.

Publication Date

2016

Publisher

American Chemical Society

Source Publication

Journal of the American Chemical Society

Source ISSN

0002-7863

Original Item ID

DOI: 10.1021/jacs.6b05480; PubMed Central: PMID: 27685680

Abstract

During bacterial denitrification, two-electron reduction of N2O occurs at a [Cu44-S)] catalytic site (CuZ*) embedded within the nitrous oxide reductase (N2OR) enzyme. In this Communication, an amidinate-supported [Cu4(μ4-S)] model cluster in its one-hole (S = 1/2) redox state is thoroughly characterized. Along with its two-hole redox partner and fully reduced clusters reported previously, the new species completes the two-electron redox series of [Cu44-S)] model complexes with catalytically relevant oxidation states for the first time. More importantly, N2O is reduced by the one-hole cluster to produce N2 and the two-hole cluster, thereby completing a closed cycle for N2O reduction. Not only is the title complex thus the best structural model for CuZ* to date, but it also serves as a functional CuZ* mimic.

Comments

Accepted version. Journal of the American Chemical Society, Vol. 138, No. 40 (2016): 13107-13110. DOI. © 2016 American Chemical Society. Used with permission.

Available for download on Friday, September 29, 2017

Included in

Chemistry Commons

Share

COinS