His-163 is a stereospecific proton donor in the mechanism of d-glucosaminate-6-phosphate ammonia-lyase

FEBS Lett. 2022 Sep;596(18):2441-2448. doi: 10.1002/1873-3468.14469. Epub 2022 Aug 29.

Abstract

d-Glucosaminate-6-phosphate ammonia-lyase (DGL) catalyzes the conversion of d-glucosaminate-6-phosphate to 2-keto-3-deoxyglutarate-6-phosphate, with stereospecific protonation of C-3 of the product. The crystal structure of DGL showed that His-163 could serve as the proton donor. H163A mutant DGL is fully active in the steady-state reaction, and the pre-steady-state kinetics are very similar to those of wild-type DGL. However, H163A DGL accumulates a transient intermediate with λmax at 293 nm during the reaction that is not seen with wild-type DGL. Furthermore, NMR analysis of the reaction of H163A DGL in D2 O shows that the product is a mixture of deuterated diastereomers at C-3. These results establish that His-163 is the proton donor in the reaction mechanism of DGL.

Keywords: aminoacrylate intermediate; elimination reaction; pyridoxal-5′-phosphate; stereochemistry.

Publication types

  • Research Support, Non-U.S. Gov't
  • Research Support, N.I.H., Extramural

MeSH terms

  • Ammonia-Lyases*
  • Kinetics
  • Lyases*
  • Phosphates
  • Protons

Substances

  • Phosphates
  • Protons
  • Lyases
  • Ammonia-Lyases