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Sulfanyl stabilization of copper-bonded phenoxyls in model complexes and galactose oxidase.

Abstract：

:Integrating sulfanyl substituents into copper-bonded phenoxyls significantly alters their optical and redox properties and provides insight into the influence of cysteine modification of the tyrosine cofactor in the enzyme galactose oxidase. The model complexes [1(SR2)](+) are class II mixed-valent Cu(II)-phenoxyl-phenolate species that exhibit intervalence charge transfer bands and intense visible sulfur-aryl π → π* transitions in the energy range, which provides a greater spectroscopic fidelity to oxidized galactose oxidase than non-sulfur-bearing analogs. The potentials for phenolate-based oxidations of the sulfanyl-substituted 1(SR2) are lower than the alkyl-substituted analogs by up to ca. 150 mV and decrease following the steric trend: -S(t)Bu > -S(i) Pr > -SMe. Density functional theory calculations suggest that reducing the steric demands of the sulfanyl substituent accommodates an in-plane conformation of the alkylsulfanyl group with the aromatic ring, which stabilizes the phenoxyl hole by ca. 8 kcal mol(-1) (1 kcal = 4.18 kJ; 350 mV) through delocalization onto the sulfur atom. Sulfur K-edge X-ray absorption spectroscopy clearly indicates a contribution of ca. 8-13% to the hole from the sulfur atoms in [1(SR2)](+). The electrochemical results for the model complexes corroborate the ca. 350 mV (density functional theory) contribution of hole delocalization on to the cysteine-tyrosine cross-link to the stability of the phenoxyl radical in the enzyme, while highlighting the importance of the in-plane conformation observed in all crystal structures of the enzyme.

journal_name

Proc Natl Acad Sci U S A

journal_title

Proceedings of the National Academy of Sciences of the United States of America

authors

Verma P,Pratt RC,Storr T,Wasinger EC,Stack TD

doi

10.1073/pnas.1109931108

subject

Has Abstract

pub_date

2011-11-15 00:00:00

pages

18600-5

issue

46

eissn

0027-8424

issn

1091-6490

pii

1109931108

journal_volume

108

pub_type

杂志文章

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