Chen Lele, Tian Jinghao, Song Huaxing, Gao Zhaohua, Wei Haisheng, Wang Wenhua, Ren Wanzhong
College of Chemistry and Chemical Engineering, Yantai University Yantai 264005 Shandong China
Collaborative Innovation Center of Comprehensive Utilization of Light Hydrocarbon Resource, Yantai University Yantai 264005 Shandong China.
RSC Adv. 2020 Sep 16;10(57):34381-34386. doi: 10.1039/d0ra06515c.
Hydroformylation of olefins is one of the most important industrial processes for aldehyde production. Therein, the leaching of active metals for heterogeneous catalysts is an important issue in the hydroformylation reaction, particularly for higher olefins to produce higher alcohols. Here, different Rh/ZnO catalysts with diverse ZnO as a support were investigated and a home-made ZnO support was selected to prepare the Rh/ZnO@ZIF-8 core-shell structure catalyst, which was synthesized by the growth of ZIF-8 with ZnO as the sacrificed template to afford Zn source. Compared with the Rh/ZnO catalyst, the Rh/ZnO@ZIF-8 catalyst demonstrated a better cyclic stability in the hydroformylation of 1-dodecene. Combining the experiment and characterization results, it was concluded that the ZIF-8 shell on the Rh/ZnO catalyst effectively prevented the leaching of metal Rh into the reaction solution. Moreover, the Rh/ZnO@ZIF-8 catalyst exhibited good universality for other higher olefins. This work provides a useful guideline for immobilizing the active species in heterogeneous catalysts for the hydroformylation reaction.
烯烃氢甲酰化反应是生产醛类最重要的工业过程之一。其中，多相催化剂中活性金属的浸出是氢甲酰化反应中的一个重要问题，特别是对于生产高级醇的高级烯烃而言。在此，研究了以不同的ZnO为载体的不同Rh/ZnO催化剂，并选择了自制的ZnO载体来制备Rh/ZnO@ZIF-8核壳结构催化剂，该催化剂通过以ZnO为牺牲模板生长ZIF-8以提供锌源而合成。与Rh/ZnO催化剂相比，Rh/ZnO@ZIF-8催化剂在1-十二烯的氢甲酰化反应中表现出更好的循环稳定性。结合实验和表征结果得出结论，Rh/ZnO催化剂上的ZIF-8壳层有效地防止了金属Rh浸出到反应溶液中。此外，Rh/ZnO@ZIF-8催化剂对其他高级烯烃表现出良好的通用性。这项工作为在多相催化剂中固定用于氢甲酰化反应的活性物种提供了有用的指导。
