Lewis酸碱调控镧掺杂氧化锌催化CO_(2)转化制碳酸乙烯酯  

Lewis acid-base modulated lanthanum-doped zinc oxide catalyzed CO_(2)conversion to ethylene carbonate

作　　者：杜昌元 苏倩[2] 许振洋 付梦倩 贾松岩 董丽[2] DU Changyuan;SU Qian;XU Zhenyang;FU Mengqian;JIA Songyan;DONG Li(College of Chemical Engineering,Shenyang University of Chemical Technology,Shenyang 110142,China;Beijing Key Laboratory of Ionic Liquid Clean Process,Institute of Process Engineering,Chinese Academy of Sciences,Beijing 100190,China)

机构地区：[1]沈阳化工大学化学工程学院,辽宁沈阳110142 [2]中国科学院过程工程研究所离子液体清洁过程北京市重点实验室,北京100190

出　　处：《燃料化学学报（中英文）》2024年第3期305-312,共8页Journal of Fuel Chemistry and Technology

基　　金：国家自然科学基金(22178356,22078329,21890763)资助。

摘　　要：本研究以CO_(2)和乙二醇(EG)合成碳酸乙烯酯(EC)为目标,设计合成一系列La掺杂ZnO催化剂,可对ZnO表面Lewis酸碱性位点调控,并在无助剂条件下研究了催化剂活性。La-ZnO-1%-550℃具有最好的催化活性,在130℃、4 MPa CO_(2)、1 h条件下,EG的转化率为0.54%,EC的时空收率和选择性分别为7.326 mmol/(h·g)和99%,并具有良好的稳定性。结合对催化剂的晶体结构、形貌和表面酸碱性等分析,结果显示,La均匀分布在ZnO中空纳米片中,经过550℃煅烧的La掺杂ZnO的表面具有最多的Lewis酸碱性位点,催化剂的催化活性随中强Lewis酸碱性位点增多而升高。The massive emission of the greenhouse gas CO_(2)has caused problems such as global warming and ecological damage.How to effectively utilize CO_(2)as a resource and create economic benefits has attracted much attention in recent years.In this paper,a series of La-doped ZnO catalysts were designed and synthesized targeting the synthesis of ethylene carbonate(EC)from CO_(2)and ethylene glycol(EG),which could modulate the Lewis acid-base sites on the ZnO surface,and the catalyst activity was investigated under additive-free conditions.La-ZnO-1%-550℃had the best catalytic activity with 0.54%conversion of EG,7.326 mmol/(h∙g)and 99%space-time yield and selectivity of EC at 130℃,4 MPa CO_(2),and 1 h with good stability.Combined with the analysis of the crystal structure,morphology and surface acid-base of the catalysts,the results showed that La was uniformly distributed in the ZnO hollow nanosheets,and the surface of the La-doped ZnO calcined at 550℃had the most Lewis acid-base sites,and the catalytic activity of the catalysts increased with the increase of moderate to strong Lewis acid-base sites.

关 键 词：CO_(2) ZNO 碳酸乙烯酯 Lewis酸碱催化 

分 类 号：O643.36[理学—物理化学]