Biochemistry p. 1627 - 1647 (2019)
Update date:2022-08-15
Topics:
Rajakovich, Lauren J.
Pandelia, Maria-Eirini
Mitchell, Andrew J.
Chang, Wei-Chen
Zhang, Bo
Boal, Amie K.
Krebs, Carsten
Bollinger, J. Martin
The assignment of biochemical functions to hypothetical proteins is challenged by functional diversification within many protein structural superfamilies. This diversification, which is particularly common for metalloenzymes, renders functional annotations that are founded solely on sequence and domain similarities unreliable and often erroneous. Definitive biochemical characterization to delineate functional subgroups within these superfamilies will aid in improving bioinformatic approaches for functional annotation. We describe here the structural and functional characterization of two non-heme-iron oxygenases, TmpA and TmpB, which are encoded by a genomically clustered pair of genes found in more than 350 species of bacteria. TmpA and TmpB are functional homologues of a pair of enzymes (PhnY and PhnZ) that degrade 2-aminoethylphosphonate but instead act on its naturally occurring, quaternary ammonium analogue, 2-(trimethylammonio)ethylphosphonate (TMAEP). TmpA, an iron(II)- and 2-(oxo)glutarate-dependent oxygenase misannotated as a γ-butyrobetaine (γbb) hydroxylase, shows no activity toward γbb but efficiently hydroxylates TMAEP. The product, (R)-1-hydroxy-2-(trimethylammonio)ethylphosphonate [(R)-OH-TMAEP], then serves as the substrate for the second enzyme, TmpB. By contrast to its purported phosphohydrolytic activity, TmpB is an HD-domain oxygenase that uses a mixed-valent diiron cofactor to enact oxidative cleavage of the C-P bond of its substrate, yielding glycine betaine and phosphate. The high specificities of TmpA and TmpB for their N-trimethylated substrates suggest that they have evolved specifically to degrade TMAEP, which was not previously known to be subject to microbial catabolism. This study thus adds to the growing list of known pathways through which microbes break down organophosphonates to harvest phosphorus, carbon, and nitrogen in nutrient-limited niches.
View Morewebsite:http://www.cartoonchem.com/
Contact:+86-25-58074918
Address:Room 2109, RuiHua Business Center,315 South ZhongShan Road, Nanjing 210001, China
website:http://www.guarson.com
Contact:+86-523-88059600,+86-13805268803
Address:Room B1006,Yafang Building,Jiangyan Avenue,Jiangyan District, Taizhou City,Jiangsu,China
Jiangsu Haian Petro chemical Plant
Contact:+86-513-88902723
Address:99, Changjiang West Road, Haian County, Jiangsu
Zhejiang Sanmei Chemical Industry Co., Ltd
Contact:86-579-87633213
Address:Huchu Industrial Zone, Qingnian Rd., Wuyi County, Zhejiang Prov., China.
DANYANG ZHONGTAI TRADE CO .,LTD.
Contact:0086-511-86985511
Address:No.25,Dongfang Rd., Danyang City.Jiangsu P.R.China
Doi:10.1002/ejoc.201700824
(2017)Doi:10.1016/S0040-4039(01)00951-0
(2001)Doi:10.1246/cl.1996.647
(1996)Doi:10.1021/ja00033a028
(1992)Doi:10.1016/j.molstruc.2020.129733
(2021)Doi:10.1002/hlca.19670500307
(1967)