@article{404a5d3b610345549d9fd4094ee742c9,
title = "Purinyl-cobamide is a native prosthetic group of reductive dehalogenases",
abstract = "Cobamides such as vitamin B 12 are structurally conserved, cobalt-containing tetrapyrrole biomolecules that have essential biochemical functions in all domains of life. In organohalide respiration, a vital biological process for the global cycling of natural and anthropogenic organohalogens, cobamides are the requisite prosthetic groups for carbon-halogen bond-cleaving reductive dehalogenases. This study reports the biosynthesis of a new cobamide with unsubstituted purine as the lower base and assigns unsubstituted purine a biological function by demonstrating that Coα-purinyl-cobamide (purinyl-Cba) is the native prosthetic group in catalytically active tetrachloroethene reductive dehalogenases of Desulfitobacterium hafniense. Cobamides featuring different lower bases are not functionally equivalent, and purinyl-Cba elicits different physiological responses in corrinoid-auxotrophic, organohalide-respiring bacteria. Given that cobamide-dependent enzymes catalyze key steps in essential metabolic pathways, the discovery of a novel cobamide structure and the realization that lower bases can effectively modulate enzyme activities generate opportunities to manipulate functionalities of microbiomes.",
author = "Jun Yan and Meng Bi and Bourdon, {Allen K.} and Farmer, {Abigail T.} and Wang, {Po Hsiang} and Olivia Molenda and Quaile, {Andrew T.} and Nannan Jiang and Yi Yang and Yongchao Yin and Burcu {\c S}im{\c s}ir and Campagna, {Shawn R.} and Edwards, {Elizabeth A.} and L{\"o}ffler, {Frank E.}",
note = "Funding Information: We thank J. Maillard, {\'E}cole Polytechnique F{\'e}d{\'e}rale de Lausanne, France, for providing Dehalobacter restrictus strain PER-K23. We also thank R. Flick from the BioZone Mass Spectrometry facility, Toronto, for LC/MS assistance. This research was supported by a grant from the Superfund Research Program under the National Institute of Environmental Health Sciences (R01ES024294) to F.E.L., with additional support provided by the Strategic Environmental Research and Development Program (SERDP project ER-2312) to F.E.L. and by the Natural Science and Engineering Research Council of Canada (NSERC) Industrial Biocatalysis Network to E.A.E. Y. Yin acknowledges the financial support from the China-UT One-Hundred Scholars Program by the China Scholarship Council and the University of Tennessee.",
year = "2018",
month = jan,
day = "1",
doi = "10.1038/nchembio.2512",
language = "???core.languages.en_GB???",
volume = "14",
pages = "8--14",
journal = "Nature Chemical Biology",
issn = "1552-4450",
number = "1",
}