无金属组分的氮化碳材料催化CO_(2)合成碳酸丙烯酯  

Synthesis of Propylene Carbonate from CO_(2)Catalyzed by Metal-free Carbon Nitride

作　　者：孙校华 张学文 王非[1] 许杰[1] 薛冰[1] SUN Xiao-hua;ZHANG Xue-wen;WANG Fei;XU Jie;XUE Bing(School of Petrochemical Engineering,Changzhou University,Changzhou 213164,China)

机构地区：[1]常州大学石油化工学院,江苏常州213164

出　　处：《分子催化（中英文）》2024年第5期409-417,I0001,共10页Journal of Molecular Catalysis(China)

基　　金：国家自然科学基金项目(22278041);中国石油—常州大学创新联合体科技创新人才项目(CCIA2023-02)。

摘　　要：以二氰二胺为前驱体,经热聚和热剥离制备了剥离石墨相氮化碳(eg-C_(3)N_(4))材料,eg-C_(3)N_(4)再经H_(2)SO_(4)处理制得了eg-C_(3)N_(4)-S材料.采用N_(2)-吸脱附、X射线衍射、傅里叶红外光谱、X射线光电子能谱和紫外-可见漫反射等方法对材料的孔结构、化学组成等理化性质进行了表征.结果显示,热剥离有效地提高了g-C_(3)N_(4)的比表面积,而H_(2)SO_(4)处理引入了羟基.在CO_(2)和环氧丙烷环加成合成碳酸丙烯酯的催化反应中,eg-C_(3)N_(4)-S材料相较于未经H_(2)SO_(4)处理或未经热剥离的g-C_(3)N_(4)材料具有更高的催化活性.在反应压力为2.0 MPa,反应温度为140℃条件下,环氧丙烷的转化率和碳酸丙烯酯选择性分别为85%和98%.The exfoliated graphitic carbon nitride(eg-C_(3)N_(4))material was synthesized by thermal polymerization and thermal exfoliation using dicyanodiamide as a precursor,and the eg-C_(3)N_(4)-S materials were prepared by treatment of H_(2)SO_(4).The physicochemical properties,including porous structure,chemical compositions etc.,of the materials were characterized by N_(2)adsorption-desorption,XRD,FT-IR,XPS and UV-Vis spectroscopy.The characterization results showed that exfoliation effectively increased the specific surface area of g-C_(3)N_(4),while H_(2)SO_(4)treatment introduced hydroxyl group.In the catalytic reaction of cycloaddition of CO_(2)with propylene oxide to propylene carbonate,eg-C_(3)N_(4)-S showed higher catalytic activity than g-C_(3)N_(4)without H_(2)SO_(4)treatment or thermal exfoliation.Under the reaction pressure of 2.0 MPa and temperature of 140℃,the propylene oxide conversion and propylene carbonate selectivity were 85%and 98%,respectively.

关 键 词：氮化碳 环碳酸酯 CO_(2)环加成反应 

分 类 号：O643.32[理学—物理化学]