Enzyme catalysis captured using multiple structures from one crystal at varying temperatures

IUCrJ
Sam HorrellMichael A Hough

Abstract

High-resolution crystal structures of enzymes in relevant redox states have transformed our understanding of enzyme catalysis. Recent developments have demonstrated that X-rays can be used, via the generation of solvated electrons, to drive reactions in crystals at cryogenic temperatures (100 K) to generate 'structural movies' of enzyme reactions. However, a serious limitation at these temperatures is that protein conformational motion can be significantly supressed. Here, the recently developed MSOX (multiple serial structures from one crystal) approach has been applied to nitrite-bound copper nitrite reductase at room temperature and at 190 K, close to the glass transition. During both series of multiple structures, nitrite was initially observed in a 'top-hat' geometry, which was rapidly transformed to a 'side-on' configuration before conversion to side-on NO, followed by dissociation of NO and substitution by water to reform the resting state. Density functional theory calculations indicate that the top-hat orientation corresponds to the oxidized type 2 copper site, while the side-on orientation is consistent with the reduced state. It is demonstrated that substrate-to-product conversion within the crystal occurs at a lower...Continue Reading

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Citations

Mar 2, 2019·Acta Crystallographica. Section D, Structural Biology·Ali EbrahimRobin L Owen
Nov 21, 2018·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Kakali SenThomas W Keal
Aug 8, 2018·Acta Crystallographica. Section D, Structural Biology·Yohta FukudaTsuyoshi Inoue
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Jun 8, 2021·Chemical Science·Michael A HoughS Samar Hasnain
Dec 5, 2018·Journal of Chemical Theory and Computation·You LuThomas W Keal
Aug 30, 2021·Current Opinion in Structural Biology·Michael A Hough, Robin L Owen
Oct 5, 2021·Acta Crystallographica. Section D, Structural Biology·Gabriela C Schröder, Flora Meilleur

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Methods Mentioned

BETA
X-ray

Software Mentioned

MSOX
XDS
Molden
PyMOL
REFMAC
AIMLESS
DL
FIND
ORCA
ds2

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