不同晶相结构ZrO2负载铜基催化剂用于二乙醇胺脱氢反应

ZrO2 with Different Crystal Structure Supported Cu Catalysts for the Dehydrogenation of Diethanolamine

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^+/Cu^0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,反应时间为2.5 h,亚氨基二乙酸收率为97.64%。

ZrO2 carriers with different crystal structure including monoclinic phase(m-ZrO2),tetragonal phase(t-ZrO2)and amorphous phase(a-ZrO2)were prepared.Subsequently,Cu/m-ZrO2,Cu/t-ZrO2,and Cu/a-ZrO2 catalysts were prepared by sedimentation method and then were applied to synthesize iminodiacetic acid by the dehydrogenation of diethanolamine.The structures of the catalysts were characterized by XRD,nitrogen-physical adsorption desorption,XPS,H2-TPR and CO2-TPD.The results showed that Cu/m-ZrO2 catalyst’s interface was more conducive to the stable existence of Cu^+/Cu^0,with more alkaline sites and better oxidation resistance.In the dehydrogenation of diethanolamine,Cu/m-ZrO2 catalyst had better performance,the reaction time was 2.5 h,and the yield of iminodiacetic acid was 97.64%.