6-sulfate modified N-acetylglucosamine (6-sulfo-GlcNAc) is often found as part of many biologically important carbohydrate epitopes such as 6-sulfo-Le(X). In these epitopes, the 6-sulfo-GlcNAc moiety is extended by a galactose sugar in a β1-4 linkage. The β4GalT1 enzyme transfers galactose (Gal) from UDP-Gal to N-acetylglucosamine (GlcNAc) in the presence of manganese. Here we report that the β4GalT1 enzyme transfers Gal to the 6-sulfo-GlcNAc and 4-methylumbelliferyl-6-sulfo-N-acetyl-β-D-glucosaminide (6-sulfo-βGlcNAc-MU) acceptor substrates, although with very low efficiency. To understand the effect that the 6-sulfate group on the GlcNAc acceptor has on the catalytic activity of the β4GalT1 molecule, we have determined the crystal structure of the catalytic domain of bovine β4GalT1 mutant enzyme M344H-β4GalT1 complex with the 6-sulfo-GlcNAc molecule. In the crystal structure, the 6-sulfo-GlcNAc is bound to the protein in a way that is similar to the GlcNAc molecule. However, the 6-sulfate group engages in additional interactions with the hydrophobic region, residues 276-285, of the protein molecule, and this group is found wedged between the aromatic side chains of Phe-280 and Trp314 residues. Since the side chain of the Trp314 residue undergoes conformational changes during the catalytic cycle of the enzyme, molecular interaction between Trp314 and the 6-sulfate group might hinder this conformational change. Therefore, the lack of a favorable binding environment, together with hindrance to the conformational changes, might be responsible for the poor catalytic activity.

译文

6-硫酸盐修饰的N-乙酰葡萄糖胺 (6-sulfo-GlcNAc) 通常被发现为许多生物学上重要的碳水化合物表位的一部分,例如6-sulfo-Le(X)。在这些表位中,6-sulfo-GlcNAc部分由 β1-4键的半乳糖糖延伸。在锰存在下,β4GalT1酶将半乳糖 (Gal) 从UDP-Gal转移到N-乙酰葡萄糖胺 (GlcNAc)。在这里,我们报告了 β4GalT1酶将Gal转移到6-sulfo-GlcNAc和4-methylumbelliferyl-6-sulfo-N-acetyl-β-D-glucosaminide (6-sulfo-βGlcNAc-MU) 受体底物上,尽管效率很低。为了了解GlcNAc受体上的6-硫酸盐基团对 β4GalT1分子的催化活性的影响,我们确定了牛 β4GalT1突变酶M344H-β4GalT1与6-sulfo-GlcNAc分子的催化结构域的晶体结构。在晶体结构中,6-磺基-GlcNAc以类似于GlcNAc分子的方式与蛋白质结合。然而,6-硫酸盐基团与蛋白质分子的疏水区域276-285残基进行另外的相互作用,并且发现该基团楔入Phe-280和Trp314残基的芳族侧链之间。由于Trp314残基的侧链在酶的催化循环过程中发生构象变化,因此Trp314与6-硫酸盐基团之间的分子相互作用可能会阻碍这种构象变化。因此,缺乏良好的结合环境以及对构象变化的阻碍,可能是导致催化活性差的原因。

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