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One-pot template-free preparation of mesoporous MgO-ZrO2 catalyst for the synthesis of dipropyl carbonate
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2018-02-14 , DOI: 10.1016/j.apcata.2018.02.013
Xuelan Zhang , Dengfeng Wang , Gongde Wu , Xiaoli Wang , Xixi Jiang , Shanfang Liu , Diangen Zhou , Dongmei Xu , Jun Gao

A series of mesoporous nano-MgO-ZrO2 with various Mg:Zr atomic ratios were prepared via simple co-precipitation process without addition of a template. It was demonstrated by XRD, N2 adsorption-desorption and TEM that these samples still kept well mesoporous structure even after calcination at 600 °C. During the preparation process, divalent Mg2+ ions could be incorporated into tetragonal ZrO2 lattice to form a solid solution. More important, the surface basic density of these catalysts closely depended on their Mg content. Then, the resulting MgO-ZrO2 catalysts were used as basic catalysts for the dipropyl carbonate (DPC) synthesis via transesterification of n-propanol and dimethyl carbonate. The relationship between the basic property of solid base and their catalytic performance was clarified in detail. Among all the materials, the catalyst with Mg:Zr atomic ratio = 0.5 showed the best catalytic performance. Under the suitable reaction conditions, the yield of DPC could reach 98.5% with 100% selectivity. In addition, based on the reusability test and catalyst characterization, this catalyst exhibited extraordinary structure stability and it could be reused at least four times without obvious loss of reactivity.



中文翻译:

一锅法无模板制备用于合成碳酸二丙酯的介孔MgO-ZrO 2催化剂

通过简单的共沉淀过程无需添加模板即可制备出一系列具有不同Mg:Zr原子比的介孔纳米MgO-ZrO 2。XRD,N 2吸附-脱附和TEM证明,即使在600°C煅烧后,这些样品仍保持良好的介孔结构。在制备过程中,可以将二价Mg 2+离子掺入四方ZrO 2晶格中以形成固溶体。更重要的是,这些催化剂的表面基本密度紧密依赖于它们的Mg含量。然后,将所得的MgO-ZrO 2催化剂用作通过n的酯交换反应合成碳酸二丙酯(DPC)的碱性催化剂-丙醇和碳酸二甲酯。详细阐明了固体碱的基本性质与其催化性能之间的关系。在所有材料中,Mg:Zr原子比= 0.5的催化剂表现出最佳的催化性能。在合适的反应条件下,DPC的收率可达98.5%,选择性为100%。另外,基于可重复使用性测试和催化剂表征,该催化剂表现出非凡的结构稳定性,并且可以重复使用至少四次而不会明显降低反应性。

更新日期:2018-02-14
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