Structural insights into the function of a thermostable copper-containing nitrite reductase

Fukuda, Y; Tse, KM; Lintuluoto, M; Fukunishi, Y; Mizohata, E; Matsumura, H; Takami, H; Nojiri, M; Inoue, T

HERO ID

2232089

Reference Type

Journal Article

Year

2014

Language

English

PMID

24293549

HERO ID 2232089
In Press No
Year 2014
Title Structural insights into the function of a thermostable copper-containing nitrite reductase
Authors Fukuda, Y; Tse, KM; Lintuluoto, M; Fukunishi, Y; Mizohata, E; Matsumura, H; Takami, H; Nojiri, M; Inoue, T
Journal Journal of Biochemistry
Volume 155
Issue 2
Page Numbers 123-135
Abstract Copper-containing nitrite reductase (CuNIR) catalyzes the reduction of nitrite (NO(-)2) to nitric oxide (NO) during denitrification. We determined the crystal structures of CuNIR from thermophilic gram-positive bacterium, Geobacillus thermodenitrificans (GtNIR) in chloride- and formate-bound forms of wild type at 1.15 Å resolution and the nitrite-bound form of the C135A mutant at 1.90 Å resolution. The structure of C135A with nitrite displays a unique η(1)-O coordination mode of nitrite at the catalytic copper site (T2Cu), which has never been observed at the T2Cu site in known wild-type CuNIRs, because the mobility of two residues essential to catalytic activity, Asp98 and His244, are sterically restricted in GtNIR by Phe109 on a characteristic loop structure that is found above Asp98 and by an unusually short CH-O hydrogen bond observed between His244 and water, respectively. A detailed comparison of the WT structure with the nitrite-bound C135A structure implies the replacement of hydrogen-bond networks around His244 and predicts the flow path of protons consumed by nitrite reduction. On the basis of these observations, the reaction mechanism of GtNIR through the η(1)-O coordination manner is proposed.
Doi 10.1093/jb/mvt107
Pmid 24293549
Wosid WOS:000330895000007
Is Certified Translation No
Dupe Override No
Is Public Yes
Language Text English
Keyword Metallo; Enzyme; Oxidation-Reduction; Enzyme; Copper; Metals; X-ray Crystallography; Methods; Thermostable enzyme