Heterometallic metal-organic framework-templated synthesis of porous Co3O4/ZnO nanocage catalysts for the carbonylation of glycerol
Heterometallic metal-organic framework-templated synthesis of porous Co3O4/ZnO nanocage catalysts for the carbonylation of glycerol
复制标题
异金属金属有机骨架模板合成多孔Co3O4/ZnO纳米笼催化剂用于甘油羰基化
DOI：
10.1016/j.jssc.2017.08.035
复制
发表时间：
2017
影响因子：
3.3
通讯作者：
Zheng Lansun
中科院分区：
文献类型：
--
作者：
Lu Yinyun;Jiang Yating;Zhou Qi;Li Yunmei;Chen Luning;Kuang Qin;Xie Zhaoxiong;Zheng Lansun
碳酸甘油酯（GLC）的高效合成近年来因其在减少生物柴油生产中过量甘油方面的重要意义以及在多个工业领域的良好应用而受到广泛关注。然而，由于缺乏高性能固体催化剂，在多相催化过程中实现甘油制 GLC 的高转化率和高选择性仍然是一个挑战。在此，通过简单的异金属金属有机骨架（MOF）模板合成路线成功制备了由充分混合的 Co3O4 和 ZnO 纳米晶体组成的高度多孔的纳米笼催化剂。得益于高孔隙率以及Co3O4和ZnO之间的协同效应，与单组分催化剂相比，所制备的复合催化剂在甘油与尿素的羰基化反应中表现出显着提高的GLC生产效率。 Co50Zn50-350催化剂的GLC产率达到85.2%，转化率93.3%，GLC选择性接近91%，催化性能优于大多数非均相催化剂。更重要的是，所提出的异金属MOF的模板化合成策略有利于催化剂组成和表面结构的调节，因此可以潜在地扩展到其他金属氧化物复合催化剂的定制中。
The efficient synthesis of glycerol carbonate (GLC) has recently received great attention due to its significance in reducing excess glycerol in biodiesel production as well as its promising applications in several industrial fields. However, the achievement of high conversion and high selectivity of GLC from glycerol in heterogeneous catalytic processes remains a challenge due to the absence of high-performance solid catalysts. Herein, highly porous nanocage catalysts composed of well-mixed Co3O4and ZnO nanocrystals were successfully fabricated via a facile heterometallic metal-organic framework (MOF)-templated synthetic route. Benefiting from a high porosity and the synergistic effect between Co3O4and ZnO, the as-prepared composite catalysts exhibited a significantly enhanced production efficiency of GLC in the carbonylation reaction of glycerol with urea compared to the single-component counterparts. The yield of GLC over the Co50Zn50-350 catalyst reached 85.2%, with 93.3% conversion and near 91% GLC selectivity, and this catalytic performance was superior to that over most heterogeneous catalysts. More importantly, the proposed templated synthetic strategy of heterometallic MOFs facilitates the regulation of catalyst composition and surface structure and can therefore be potentially extended in the tailoring of other metal oxide composite catalysts.