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CH···S hydrogen bonds drive molecular recognition of ergothioneine by the microbial transporter

Legg, K. A.; Gonzalez-Gutierrez, G.; Edmonds, K. A.; Shushkov, P. G.; Giedroc, D. P.

2025-07-31 biochemistry
10.1101/2025.07.28.667264 bioRxiv
Show abstract

Many bacteria harbor an ATP-binding cassette (ABC) transporter named EgtU specific for the human dietary antioxidant and 2-thioimidazole-containing low molecular weight thiol ergothioneine (ET). How the solute binding domain, EgtUC, discriminates among ET and other similar molecules is unknown. Here, we use a "chimeric" mutagenesis strategy and two distantly related EgtUCs from Streptococcus pneumoniae and Helicobacter pylori to show that a suite of EgtUC alkyl CH***S hydrogen bonds to the ET thione S atom are central determinants of molecular recognition. Small perturbations in CH***S distance and angle give rise to sharply attenuated transport-competent ET-bound "closed" state lifetimes and increased motional disorder in the binding pocket, not around the S atom itself, but distally in weakening NH***O hydrogen bonds. This is, to our knowledge, the first work to describe the impact of alkyl CH***S H-bonding in a biological protein-ligand complex in water.

Published in Science Advances (predicted rank #4) · training set

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