Purinyl-cobamide is a native prosthetic group of reductive dehalogenases
Abstract
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.
- Authors:
-
- 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)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1471874
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Chemical Biology
- Additional Journal Information:
- Journal Volume: 14; Journal Issue: 1; Journal ID: ISSN 1552-4450
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
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., and Löffler, Frank E. Purinyl-cobamide is a native prosthetic group of reductive dehalogenases. United States: N. p., 2017.
Web. doi:10.1038/nchembio.2512.
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. Purinyl-cobamide is a native prosthetic group of reductive dehalogenases. United States. https://doi.org/10.1038/nchembio.2512
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., and Löffler, Frank E. Mon .
"Purinyl-cobamide is a native prosthetic group of reductive dehalogenases". United States. https://doi.org/10.1038/nchembio.2512. https://www.osti.gov/servlets/purl/1471874.
@article{osti_1471874,
title = {Purinyl-cobamide is a native prosthetic group of reductive dehalogenases},
author = {Yan, Jun and Bi, Meng and Bourdon, Allen K. and Farmer, Abigail T. and Wang, Po -Hsiang and Molenda, Olivia and Quaile, Andrew T. and Jiang, Nannan and Yang, Yi and Yin, Yongchao and Şimşir, Burcu and Campagna, Shawn R. and Edwards, Elizabeth A. and Löffler, Frank E.},
abstractNote = {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.},
doi = {10.1038/nchembio.2512},
journal = {Nature Chemical Biology},
number = 1,
volume = 14,
place = {United States},
year = {Mon Nov 06 00:00:00 EST 2017},
month = {Mon Nov 06 00:00:00 EST 2017}
}
Web of Science
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