QM/MM Studies Reveal How Substrate-Substrate and Enzyme-Substrate Interactions Modulate Retaining Glycosyltransferases Catalysis and Mechanism. 2015

Hansel Gómez, and Fernanda Mendoza, and José M Lluch, and Laura Masgrau
Institut de Biotecnologia i de Biomedicina (IBB), Universitat Autònoma de Barcelona, Bellaterra (Barcelona), Spain; Departament de Química, Universitat Autònoma de Barcelona, Bellaterra (Barcelona), Spain. Electronic address: Laura.Masgrau@uab.cat.

Glycosyltransferases (GTs) catalyze the biosynthesis of glycosidic linkages by transferring a monosaccharide from a nucleotide sugar donor to an acceptor substrate, and they do that with exquisite regio- and stereospecificity. Retaining GTs act with retention of the configuration at the anomeric carbon of the transferred sugar. Their chemical mechanism has been under debate for long as conclusive experimental data to confirm the mechanism have been elusive. In the past years, quantum mechanical/molecular mechanical (QM/MM) calculations have shed light on the mechanistic discussion. Here, we review the work carried out in our group investigating three of these retaining enzymes (LgtC, α3GalT, and GalNAc-T2). Our results support the controversial front-side attack mechanism as the general mechanism for most retaining GTs. The latest structural data are in agreement with these findings. QM/MM calculations have revealed how enzyme-substrate and substrate-substrate interactions modulate the transfer reaction catalyzed by these enzymes. Moreover, they provide an explanation on why in some cases a strong nucleophilic residue is found on the β-face of the sugar, opening the door to a shift toward a double-displacement mechanism.

UI MeSH Term Description Entries
D007700 Kinetics The rate dynamics in chemical or physical systems.
D009005 Monosaccharides Single chain carbohydrates that are the most basic units of CARBOHYDRATES. They are typically colorless crystalline substances with a sweet taste and have the same general formula CnH2nOn. Monosaccharide,Simple Sugar,Simple Sugars,Sugar, Simple,Sugars, Simple
D011789 Quantum Theory The theory that the radiation and absorption of energy take place in definite quantities called quanta (E) which vary in size and are defined by the equation E Quantum Theories,Theories, Quantum,Theory, Quantum
D005700 Galactosyltransferases Enzymes that catalyze the transfer of galactose from a nucleoside diphosphate galactose to an acceptor molecule which is frequently another carbohydrate. EC 2.4.1.-. Galactosyltransferase
D006801 Humans Members of the species Homo sapiens. Homo sapiens,Man (Taxonomy),Human,Man, Modern,Modern Man
D006900 Hydroxylation Placing of a hydroxyl group on a compound in a position where one did not exist before. (Stedman, 26th ed) Hydroxylations
D000097763 Polypeptide N-acetylgalactosaminyltransferase Family of enzymes that catalyze the formation of GalNAcAlpha1-serine/threonine linkages in glycoproteins. Galactosylgalactosylglucosylceramide beta-D-acetylgalactosaminyltransferase,Globoside Synthase,Globoside beta GalNAc Transferase,Protein-UDPacetylgalactosaminyltransferase,(1-3)-N-acetyl-beta-galactosaminyltransferase,(1-4)-N-acetyl-beta-D-galactosaminyltransferase,4-GalNActransferase,GalNAc-T1,GalNAc-T10,GalNAc-T2,GalNAc-T3,GalNAc-T4,GalNAc-T5,GalNAc-T8,GalNAc-transferase,GalNAcT-1,GalNAcT-2,GalNAcT-4,GalNAcT-8,UDP-GPAGAT,UDP-GalNAc-beta-galactose beta 1,4-N-acetylgalactosaminyltransferase,UDP-GalNAc-polypeptide N-acetylgalactosaminyltransferase,UDP-N-acetyl-D-galactosamine polypeptide N-acetylgalactosaminyltransferase-T4,UDP-N-acetylgalactosamine mucin transferase,UDP-N-acetylgalactosamine-beta-galactose beta 1,4-N-acetylgalactosaminyltransferase,UDP-N-acetylgalactosamine-globoside beta-N-acetylgalactosaminyltransferase,UDP-N-acetylgalactosamine-globosidetriaosylceramide beta-3-N-acetylgalactosaminyltransferase,UDP-N-acetylgalactosamine-polypeptide N-acetylgalactosamine transferase,UDPacetylgalactosamine-galactosyl-galactosyl-glucosylceramide beta-N-acetyl-D-galactosaminyltransferase,UDPacetylgalactosamine-protein acetylgalactosaminyltransferase,beta-1,4-N-acetylgalactosaminyltransferase,beta-N-acetylgalactosaminyltransferase,beta1,6N-acetylgalactosaminyltransferase,polypeptide N-acetylgalactosaminyltransferase 1,polypeptide N-acetylgalactosaminyltransferase 10,polypeptide N-acetylgalactosaminyltransferase 2,polypeptide N-acetylgalactosaminyltransferase 3,polypeptide N-acetylgalactosaminyltransferase 4,polypeptide N-acetylgalactosaminyltransferase 5,polypeptide N-acetylgalactosaminyltransferase 8,pp-GalNAc-T10,ppGalNAc-T,Synthase, Globoside
D001419 Bacteria One of the three domains of life (the others being Eukarya and ARCHAEA), also called Eubacteria. They are unicellular prokaryotic microorganisms which generally possess rigid cell walls, multiply by cell division, and exhibit three principal forms: round or coccal, rodlike or bacillary, and spiral or spirochetal. Bacteria can be classified by their response to OXYGEN: aerobic, anaerobic, or facultatively anaerobic; by the mode by which they obtain their energy: chemotrophy (via chemical reaction) or PHOTOTROPHY (via light reaction); for chemotrophs by their source of chemical energy: CHEMOLITHOTROPHY (from inorganic compounds) or chemoorganotrophy (from organic compounds); and by their source for CARBON; NITROGEN; etc.; HETEROTROPHY (from organic sources) or AUTOTROPHY (from CARBON DIOXIDE). They can also be classified by whether or not they stain (based on the structure of their CELL WALLS) with CRYSTAL VIOLET dye: gram-negative or gram-positive. Eubacteria
D001426 Bacterial Proteins Proteins found in any species of bacterium. Bacterial Gene Products,Bacterial Gene Proteins,Gene Products, Bacterial,Bacterial Gene Product,Bacterial Gene Protein,Bacterial Protein,Gene Product, Bacterial,Gene Protein, Bacterial,Gene Proteins, Bacterial,Protein, Bacterial,Proteins, Bacterial
D013237 Stereoisomerism The phenomenon whereby compounds whose molecules have the same number and kind of atoms and the same atomic arrangement, but differ in their spatial relationships. (From McGraw-Hill Dictionary of Scientific and Technical Terms, 5th ed) Molecular Stereochemistry,Stereoisomers,Stereochemistry, Molecular,Stereoisomer

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