pH-Controlled Nanoparticle Catalysts for Highly Selective Tandem Henry Reaction from Mixtures.
pH-Controlled Nanoparticle Catalysts for Highly Selective Tandem Henry Reaction from Mixtures.
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DOI：
10.1021/acscatal.0c03468
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发表时间：
2020-12-04
期刊：
影响因子：
12.9
通讯作者：
Zhao Y
中科院分区：
文献类型：
--
作者：
Bose I;Zhao Y
大自然具有使用酶催化剂将复杂的生物混合物选择性转化为所需产物的显著能力。我们报道了通过交联胶束内的分子印迹制备纳米催化剂。这些催化剂对目标底物具有高度选择性，即使在碱性条件下也能选择性水解反应性较低的缩醛。它们的催化活性和选择性可通过对活性中心的合理后修饰来调节。这些性质使得纳米颗粒催化剂能够在串联脱保护/亨利反应中从四组分缩醛混合物生产所需的β-硝基醇，该反应在两个步骤中需要不相容的酸性和碱性催化剂。
Nature has a remarkable ability to perform selective transformation of complex biological mixtures into desired products using enzymatic catalysts. We report the preparation of nanoparticle catalysts through molecular imprinting within cross-linked micelles. These catalysts were highly selective for their targeted substrates and could selectively hydrolyze less reactive acetals over more reactive ones even under basic conditions. Their catalytic activity and selectivity were tunable through rational postmodification of the active site. These properties enabled the nanoparticle catalysts to produce the desired β-nitro alcohol from a four-component acetal mixture in a tandem deprotection/Henry reaction that required incompatible acidic and basic catalysts in the two steps.
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