Issue 31, 2018

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

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.

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

Supplementary files

Article information

Article type
Paper
Submitted
29 mar 2018
Accepted
14 jun 2018
First published
18 jul 2018
This article is Open Access
Creative Commons BY-NC license

Dalton Trans., 2018,47, 10463-10472

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

H. Lumpe, A. Pol, H. J. M. Op den Camp and L. J. Daumann, Dalton Trans., 2018, 47, 10463 DOI: 10.1039/C8DT01238E

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