Two-dimensional (2D) molecular sieves with highly dispersed active centers have great potential as catalysts for the transformation of bulky biomass derivatives owing to the ease of molecular diffusion and the deactivation resistance by coke deposition. Here, we report a single-step preparation of a 2D Lewis acidic zincosilicate delaminated MWW layer (Zn-DML) and Lewis–Brønsted acidic ZnAl-DML catalysts by a simple hydrothermal treatment of a borosilicate MWW precursor with Zn and/or Al precursor solutions. Both framework Zn and ultra-small Zn clusters are highly dispersed in Zn-DML, while framework Al species prevail over Zn in ZnAl-DML catalysts. Zn-DML catalysts are more delaminated than ZnAl-DML catalysts. Density functional theory calculations show that heteroatom-substituted 2D MWW layers are more stable than their 3D analogues, and Al-containing systems are more stable than Zn. Lewis acidic Zn-DML was selective for fructose, whereas Lewis–Brønsted acidic ZnAl-DML catalysts were selective for 5-hydroxymethylfurfural in the catalytic glucose conversion.

中文翻译：

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用于葡萄糖催化转化的锌和铝硅酸盐分层 MWW 层的一步制备

具有高度分散的活性中心的二维 (2D) 分子筛由于易于分子扩散和焦炭沉积而具有抗失活性，因此具有作为大块生物质衍生物转化催化剂的巨大潜力。在这里，我们报告了通过用锌和/或铝前体溶液对硼硅酸盐 MWW 前体进行简单的水热处理，一步制备 2D 路易斯酸性锌硅酸盐分层 MWW 层（Zn-DML）和 Lewis-Brønsted 酸性 ZnAl-DML 催化剂. 框架 Zn 和超小 Zn 簇均高度分散在 Zn-DML 中，而框架 Al 物种在 ZnAl-DML 催化剂中优于 Zn。Zn-DML 催化剂比 ZnAl-DML 催化剂分层更多。密度泛函理论计算表明，杂原子取代的 2D MWW 层比它们的 3D 类似物更稳定，和含铝系统比锌更稳定。Lewis酸性Zn-DML对果糖具有选择性，而Lewis-Brønsted酸性ZnAl-DML催化剂在催化葡萄糖转化中对5-羟甲基糠醛具有选择性。