Zr_(x)Ce_(1-x)O_(2)/NC催化CO_(2)和苯乙烯⁃锅法制环碳酸酯  

One⁃Pot Synthesis of Cyclo⁃Carbonate from Styrene and CO_(2)over the Zr_(x)Ce_(1-x)O_(2)/NC Catalyst

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作  者:周钰淼 梁栋[1] 姚悦华 武越 赵婷 朱娜[3] ZHOU Yumiao;LIANG Dong;YAO Yuehua;WU Yue;ZHAO Ting;ZHU Na(School of Chemistry and Chemical Engineering,North University of China,Taiyuan 030051,China;Shanxi Xinhua Chemical Defense Equipment Research Institute Co.,Ltd.,Taiyuan 030008,China;School of Environmental and Resource Sciences,Shanxi University,Taiyuan 030006,China)

机构地区:[1]中北大学化学与化工学院,山西太原030051 [2]山西新华化学防护设备研究所,山西太原030008 [3]山西大学环境与资源学院,山西太原030006

出  处:《中北大学学报(自然科学版)》2024年第2期229-238,共10页Journal of North University of China(Natural Science Edition)

基  金:国家自然科学基金资助项目(22176117);山西省自然科学基金资助项目(201901D111171)。

摘  要:CO_(2)与烯烃转化为环碳酸酯是当前一种有效的固碳策略,为此设计了一种掺氮多孔碳负载锆铈双金属(Zr_(x)Ce_(1-x)O_(2)/NC)催化剂。通过X射线衍射(XRD)、扫描电子显微镜(SEM)、N_(2)-吸附、CO_(2)和NH_(3)程序升温脱附(CO_(2)-TPD和NH_(3)-TPD)等表征了催化剂的形貌、物相、孔结构以及酸碱两性特征。结果表明,该催化剂可在无卤条件下催化CO_(2)和苯乙烯一锅法制备环碳酸酯,特别是Zr_(0.75)Ce_(0.25)O_(2)/NC在2 MPa CO_(2)下,采用80℃/8 h和150℃/8 h分段工艺,实现了74.87%的转化率和80.43%的环碳酸酯选择性,这归因于氧化铈(CeO_(2))和氧化锆(ZrO_(2))在碳载体上的均匀分散,以及丰富的酸-碱性位点协同作用。The conversion of CO_(2)and olefin to cyclo-carbonate is one of effective carbon-immobilizing strategies.The zirconium-cerium bimetallic catalysts supported on the nitrogen-doped porous carbon(ZrxCe1-xO_(2)/NC)were designed and prepared.Their morphology,crystal,pore structure and acid-base characters of the catalysts were monitored by X-Ray Diffraction(XRD),scanning electron microscope(SEM),N_(2)adsorption-desorption isotherm(N_(2)-adsorption),CO_(2)-temperature program desorption(CO_(2)-TPD)and NH_(3)-temperature program desorption(NH_(3)-TPD).The results show that the catalyst can catalyse the one-pot synthesis of cyclo-carbonate by CO_(2)and styrene with halogen-free conditions.The Zr_(0.75)Ce_(0.25)O_(2)/NC show the best conversion of 74.87%and selectivity of 80.43%under 2 MPa CO_(2)through a bi-period of 80℃/8 h and 150℃/8 h.This is attributed to the uniform dispersion of CeO_(2)and ZrO_(2)on the carbon support,as well as the synergistic effect of acid-base sites.

关 键 词:CO_(2) 苯乙烯 CeO_(2) ZrO_(2) 多孔碳 环碳酸酯 

分 类 号:TQ134.1[化学工程—无机化工]

 

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