不同晶相结构ZrO2负载铜基催化剂用于二乙醇胺脱氢反应

Different phase structure of the ZrO2 supported Cu catalysts for Diethanola-mine Dehydrogenation

摘要:

通过制备不同晶相结构〔单斜相（m-ZrO2）、四方相（t-ZrO2）和无定型（a-ZrO2）〕ZrO2载体，再通过沉积沉淀法制得Cu/m-ZrO2、Cu/t-ZrO2和Cu/a-ZrO2催化剂，分别用于催化二乙醇胺脱氢合成亚氨基二乙酸反应。采用XRD、氮气-物理吸附脱附、XPS、H2-TPR、CO2-TPD对催化剂的结构进行了表征。结果表明，Cu/m-ZrO2催化剂界面更加有利于Cu+/Cu0稳定存在，具有更多的碱性位点，且抗氧化性较好。在二乙醇胺脱氢反应中，Cu/m-ZrO2催化剂性能最好，反应时间由5 h左右缩短至2.5 h，亚氨基二乙酸收率为97.64%。

Abstract:

ZrO2 carriers with different crystalline phase structures were prepared, including monoclinic phase (m-ZrO2), tetragonal phase (t-ZrO2) and amorphous phase (a-ZrO2), then Cu/m-ZrO2, Cu/t-ZrO2, and Cu/a-ZrO2 catalysts were prepared by sedimentation method and applying for synthesis of iminodiacetic acid by dehydrogenation of diethanolamine to testing theirs performance. The structures of the catalysts were characterized by XRD, Nitrogen-physical adsorption desorption, XPS, H2-TPR and CO2-TPD. The results show that Cu/ m-ZrO2 catalysts interface is more conducive to the stable existence of Cu+/Cu0, with more alkaline sites and better oxidation resistance. In the dehydrogenation reaction of diethanolamine, Cu/m-ZrO2 catalyst had better performance, the reaction time was reduced from 5 h to 2.5 h, and the yield of iminodiacetic acid was 97.64%.