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首页> 外文期刊>ACS applied materials & interfaces >Water-Tolerant DUT-Series Metal–Organic Frameworks: A Theoretical–Experimental Study for the Chemical Fixation of CO2 and Catalytic Transfer Hydrogenation of Ethyl Levulinate to γ-Valerolactone
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Water-Tolerant DUT-Series Metal–Organic Frameworks: A Theoretical–Experimental Study for the Chemical Fixation of CO2 and Catalytic Transfer Hydrogenation of Ethyl Levulinate to γ-Valerolactone

机译：耐水DUT系列金属 - 有机框架：对乙基乙基乙基乙基乙基乙基乙基催化转移氢化的理论实验研究

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A series of highly thermally and hydrolytically stable porous solids with intriguing properties of zirconium- and hafnium-based metal–organic frameworks (MOFs) [Dresden University of Technology (DUT) series] was synthesized. The DUT MOFs were found to be effective catalysts for both epoxide–CO_(2) cycloaddition reactions and the catalytic transfer hydrogenation (CTH) of ethyl levulinate (EL). In particular, 12-connected DUT-52(Zr) showed higher catalytic activity than eight- and six-connected catalysts in the synthesis of cyclic carbonates as well as in the production of γ-valerolactone (GVL). The secondary building unit connectivity, coexistence of a moderate number of acidic and basic sites, Brunauer–Emmett–Teller surface area, and combined effects of the pores of the MOFs seem to influence the catalytic activity. The reaction mechanism for the DUT-52(Zr)-mediated cycloaddition reaction of CO_(2) and the CTH reactions were investigated in detail by using periodic density functional theory calculations. To the best of our knowledge, this is the first detailed computational study for the formation of GVL from EL by using MOF as the catalyst. In addition, grand canonical Monte Carlo simulations predicted the strong interaction of CO_(2) molecules with the DUT-52(Zr) framework. Remarkably, the DUT-series catalysts possess extraordinary tolerance toward water. Further, DUT-52(Zr) is recyclable and is an efficient catalyst for cycloaddition and CTH reactions for at least five uses without obvious reductions in the activity or structural integrity.
机译：合成了一系列高度热和水解稳定的多孔固体，具有锆和铪的金属 - 有机框架（MOFS）的有趣性能[德累斯顿理工大学（DUT）系列]。发现DUT MOFS为环氧化物-CO_（2）环加成反应和乙基乙酰乙酰乙酸（EL）的催化转移氢化（CTH）是有效催化剂。特别地，12-连接的DUT-52（Zr）在合成环状碳酸盐以及γ-戊内酯（GV1）的生产中，催化活性高于八六和六个连接的催化剂。二次建筑单元连接，适度数量的酸性和基本位点的共存，Brunauer-Emmett-extreser表面积，以及MOF的孔的组合效果似乎影响了催化活性。通过使用周期性密度的功能理论计算，详细研究了DUT-52（ZR）介导的环加入反应的反应机理和CTH反应的反应。据我们所知，这是通过使用MOF作为催化剂从EL形成GV1的第一个详细的计算研究。此外，Grand Canonical Monte Carlo模拟预测CO_（2）分子与DUT-52（ZR）框架的强相互作用。值得注意的是，DUT系列催化剂对水具有非凡的耐受性。此外，DUT-52（ZR）可回收，是循环加固和第四次反应的有效催化剂，至少有五种用途，而无明显减少活性或结构完整性。

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