Impact of the lanthanide contraction on the activity of a lanthanide-dependent methanol dehydrogenase - a kinetic and DFT study

Dalton Transactions : an International Journal of Inorganic Chemistry
Henning LumpeLena J Daumann

Abstract

Interest in the bioinorganic chemistry of lanthanides is growing rapidly as more and more lanthanide-dependent bacteria are being discovered. Especially the earlier lanthanides have been shown to be preferentially utilized by bacteria that need these Lewis acids as cofactors in their alcohol dehydrogenase enzymes. Here, we investigate the impact of the lanthanide ions lanthanum(iii) to lutetium(iii) (excluding Pm) on the catalytic parameters (vmax, KM, kcat/KM) of a methanol dehydrogenase (MDH) isolated from Methylacidiphilum fumariolicum SolV. Kinetic experiments and DFT calculations were used to discuss why only the earlier lanthanides (La-Gd) promote high MDH activity. Impact of Lewis acidity, coordination number preferences, stability constants and other properties that are a direct result of the lanthanide contraction are discussed in light of the two proposed mechanisms for MDH.

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Citations

Feb 2, 2019·Science·Thibault Cheisson, Eric J Schelter
Apr 25, 2019·Chembiochem : a European Journal of Chemical Biology·Emily R FeatherstonJoseph A Cotruvo
Jun 11, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Thaige P GompaHenry S La Pierre
May 6, 2020·The Journal of Biological Chemistry·Nathan M GoodN Cecilia Martinez-Gomez
May 6, 2020·Chemistry : a European Journal·Mario PrejanòTiziana Marino
Jan 18, 2019·Molecular Microbiology·Andrea M OchsnerJulia A Vorholt
Dec 5, 2020·Acta Crystallographica. Section C, Structural Chemistry·Henning LumpeLena J Daumann
Feb 7, 2021·FEMS Microbiology Ecology·Paula Roszczenko-JasińskaRenata Matlakowska
Feb 20, 2021·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Pedro D Sarmiento-Pavía, Martha E Sosa-Torres
Apr 25, 2021·Applied and Environmental Microbiology·Carl-Eric WegnerKirsten Küsel
Jun 3, 2021·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Irena KostovaVasile Chiş
Sep 27, 2020·Biochimica Et Biophysica Acta. Molecular Cell Research·Emily R Featherston, Joseph A Cotruvo
Feb 7, 2019·Journal of the American Chemical Society·Joseph A MattocksJoseph A Cotruvo

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Software Mentioned

KaleidaGraph
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