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Mechanistic insights into the key marine dimethylsulfoniopropionate synthesis enzyme DsyB/DSYB

mLife 2022年第2期1卷 114-130页

作者： Chun-Yang Li Jason C.Crack Simone Newton-Payne Andrew R.J.Murphy Xiu-Lan Chen Benjamin J.Pinchbeck Shun Zhou Beth T.Williams Ming Peng Xiao-Hua Zhang Yin Chen Nick E.Le Brun Jonathan D.Todd Yu-Zhong Zhang Frontiers Science Center for Deep Ocean Multispheres and Earth System College of Marine Life SciencesOcean University of ChinaQingdaoChina State Key Laboratory of Microbial Technology Marine Biotechnology Research CenterShandong UniversityQingdaoChina Laboratory for marine Biology and Biotechnology Pilot National Laboratory for Marine Science and TechnologyQingdaoShandongChina School of Chemistry Centre for Molecular and Structural BiochemistryUniversity of East AngliaNorwich Research ParkNorwichUK School of Biological Sciences University of East AngliaNorwichUK School of Life Sciences University of WarwickCoventryUK

marine algae and bacteria produce approximately eight billion tonnes of the organosulfur molecule dimethylsulfoniopropionate(DMSP)in Earth's surface oceans *** is an antistress compound and,once released into the environment,a major nutrient,signaling molecule,and source of climate-active *** methionine transamination pathway for DMSP synthesis is used by most known DMSP-producing algae and *** S-directed S-adenosylmethionine(SAM)-dependent 4-methylthio-2-hydroxybutyrate(MTHB)S-methyltransferase,encoded by the dsyB/DSYB gene,is the key enzyme of this pathway,generating S-adenosylhomocysteine(SAH)and 4-dimethylsulfonio-2-hydroxybutyrate(DMSHB).DsyB/DSYB,present in most haptophyte and dinoflagellate algae with the highest known intracellular DMSP concentrations,is shown to be far more abundant and transcribed in marine environments than any other known S-methyltransferase gene in DMSP synthesis ***,we demonstrate in vitro activity of the bacterial DsyB enzyme from Nisaea denitrificans and provide its crystal structure in complex with SAM and SAH-MTHB,which together provide the first important mechanistic insights into a DMSP synthesis *** and mutational analyses imply that DsyB adopts a proximity and desolvation mechanism for the methyl transfer *** analysis suggests that this mechanism may be common to all bacterial DsyB enzymes and also,importantly,eukaryotic DSYB enzymes from e.g.,algae that are the major DMSP producers in Earth's surface oceans.

关键词： catalytic mechanism DMSP synthesis marine sulfur cycle S-methyltransferase

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