Purinyl-cobamide is a native prosthetic group of reductive dehalogenases

Yan, Jun; Bi, Meng; Bourdon, Allen K.; Farmer, Abigail T.; Wang, Po -Hsiang; Molenda, Olivia; Quaile, Andrew T.; Jiang, Nannan; Yang, Yi; Yin, Yongchao; Şimşir, Burcu; Campagna, Shawn R.; Edwards, Elizabeth A.; Löffler, Frank E.

doi:10.1038/nchembio.2512

Title: Purinyl-cobamide is a native prosthetic group of reductive dehalogenases

Journal Article · Mon Nov 06 00:00:00 EST 2017 · Nature Chemical Biology

DOI:https://doi.org/10.1038/nchembio.2512· OSTI ID:1471874

Yan, Jun ^[1]; Bi, Meng ^[2];

^[2]; Farmer, Abigail T. ^[2];

^[3]; Molenda, Olivia ^[3]; Quaile, Andrew T. ^[3];

^[4]; Yang, Yi ^[2]; Yin, Yongchao ^[2]; Şimşir, Burcu ^[2];

^[2];

^[3];

^[4]

Univ. of Tennessee, Knoxville, TN (United States); Chinese Academy of Sciences, Liaoning (People's Republic of China); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of Tennessee, Knoxville, TN (United States)
Univ. of Toronto, Toronto, ON (Canada)
Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Here, cobamides such as vitamin B₁₂ 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.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1471874

Journal Information:: Nature Chemical Biology, Vol. 14, Issue 1; ISSN 1552-4450

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 40 works

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