Synthetic glycosidases for the precise hydrolysis of oligosaccharides and polysaccharides.
Synthetic glycosidases for the precise hydrolysis of oligosaccharides and polysaccharides.
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合成糖苷酶，用于寡糖和多糖的精确水解。
DOI：
10.1039/d0sc05338d
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发表时间：
2020-11-05
期刊：
影响因子：
8.4
通讯作者：
Zhao Y
中科院分区：
文献类型：
--
作者：
Li X;Zhao Y
糖苷酶是一类重要的用于进行聚糖选择性水解的酶。虽然聚糖原则上可以被酸性水水解，但使用非酶催化剂的高选择性水解是一个未实现的目标。在交联胶束中进行分子印迹，得到了在印迹位点含有糖结合硼氧杂环戊烯的水溶性聚合物纳米颗粒。后修饰在目标糖苷键的氧附近安装酸性基团，酸的酸度和距离系统地变化。合成的糖苷酶在热水中以高度可控的方式水解寡糖和多糖。这些催化剂不仅具有与天然酶相似的选择性分解直链淀粉，而且它们还可以被设计成具有生物催化剂所不具有的选择性。底物的选择性主要取决于活性位点内结合的糖残基，包括它们的空间取向。产物的分离通过原位透析完成，并且留下的催化剂可以多次使用而没有降解的迹象。这项工作说明了一个通用的方法来构建合成的糖苷酶从容易获得的积木通过自组装，共价捕获，和后修饰。此外，受控的、精确的一步水解是从天然可获得的碳水化合物来源制备复合聚糖的有吸引力的方法。具有糖结合活性位点和精确定位的酸性基团的合成糖苷酶在热水中选择性地水解寡糖和多糖，以在单个步骤中提供所需的糖产物。
Glycosidases are an important class of enzymes for performing the selective hydrolysis of glycans. Although glycans can be hydrolyzed in principle by acidic water, hydrolysis with high selectivity using nonenzymatic catalysts is an unachieved goal. Molecular imprinting in cross-linked micelles afforded water-soluble polymeric nanoparticles with a sugar-binding boroxole in the imprinted site. Post-modification installed an acidic group near the oxygen of the targeted glycosidic bond, with the acidity and distance of the acid varied systematically. The resulting synthetic glycosidase hydrolyzed oligosaccharides and polysaccharides in a highly controlled fashion simply in hot water. These catalysts not only broke down amylose with similar selectivities to those of natural enzymes, but they also could be designed to possess selectivity not available with biocatalysts. Substrate selectivity was mainly determined by the sugar residues bound within the active site, including their spatial orientations. Separation of the product was accomplished through in situ dialysis, and the catalysts left behind could be used multiple times with no signs of degradation. This work illustrates a general method to construct synthetic glycosidases from readily available building blocks via self-assembly, covalent capture, and post-modification. In addition, controlled, precise, one-step hydrolysis is an attractive way to prepare complex glycans from naturally available carbohydrate sources. Synthetic glycosidases with a sugar-binding active site and a precisely positioned acidic group hydrolyze oligo- and polysaccharides selectively in hot water to afford desired sugar products in a single step.
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