氧磷共掺杂二维石墨相氮化碳的制备及光催化性能  

Preparation of Oxygen-Phosphorus Co-doped Two-dimensional GraphiticCarbon Nitrides and Their Photocatalytic Performances

作　　者：刘京津 赵华[1] 李会鹏[1] 蔡天凤[1] LIU Jingjin;ZHAO Hua;LI Huipeng;CAI Tianfeng(School of Petrochemical Engineering,Liaoning Petrochemical University,Fushun 113001,Liaoning,China)

机构地区：[1]辽宁石油化工大学石油化工学院,辽宁抚顺113001

出　　处：《材料导报》2024年第21期88-94,共7页Materials Reports

基　　金：辽宁省教育厅2022年度科研项目(LJKMZ20220721)。

摘　　要：以三聚氰胺、草酸铵和磷酸铵为原料,采用超分子自组装法和热聚合法制备氧磷共掺杂的二维石墨相氮化碳(g-C_(3)N_(4)),通过X射线衍射、傅里叶变换红外光谱、X射线光电子能谱、扫描电子显微镜、透射电子显微镜、氮气吸附脱附测试、紫外-可见光漫反射光谱、荧光光谱和电化学阻抗谱等手段对催化剂进行表征,以染料罗丹明B(RhB)在可见光下的降解来评价样品的光催化性能。结果表明:氧磷共掺杂使g-C_(3)N_(4)形貌由一维柱状变为二维堆叠片状,禁带宽度变窄,电子-空穴的分离效率提高,光催化性能提升。·O_(2)^(-)、·OH和h^(+)三种活性基团协同作用使样品对罗丹明B的降解率达到92.11%,在重复使用五次后降解率仍在85%以上,具有良好的稳定性。所制备的氧磷共掺杂二维g-C_(3)N_(4)降解罗丹明B的速率常数为0.01660 min^(-1),是纯g-C_(3)N_(4)的12.39倍,是由三聚氰胺-草酸铵超分子前驱体制得的g-C_(3)N_(4)的4.54倍。The oxygen-phosphorus co-doped two-dimensional graphitic carbon nitrides(g-C_(3)N_(4)),differing in the adding amount of ammonium phosphate,were prepared by supramolecular self-assembly and thermal polymerization,and were characterized by means of XRD,FTIR,XPS,SEM,TEM,UV-vis,photoluminescent spectroscopy,BET N 2 adsorption-desorption,and electrochemical impedance spectrometry.The photocatalytic activities of the samples were also estimated by catalyzing rhodamine B(RhB)degradation under visible light irradiation.The results showed that the co-doping of oxygen-phosphorus into g-C_(3)N_(4)led to the morphology transformation from one-dimensional tubes to two-dimensional stacked sheets,the narrowing of forbidden band width,the improvement in electron-hole pairs separation efficiency,and consequently,the enhancement of photocatalytic performance.The synergistic effect of the three active groups-·O_(2)^(-)、·OHandh^(+)-resulted in the RhB degradation rate of 92.11%at initial state and of above 85%after 5-time reuse in photocatalytic performance test,which indicated a good stability.Especially,one of the prepared samples achieved a rate constant of photocatalyzed RhB degradation of 0.01660 min^(-1),which was 12.39 times and 4.54 times higher than those of the pure g-C_(3)N_(4)and of the g-C_(3)N_(4)prepared by melamine-ammonium oxalate supramolecular precursor system,respectively.

关 键 词：石墨相氮化碳(g-C_(3)N_(4)) 超分子自组装 光催化 共掺杂 

分 类 号：X703[环境科学与工程—环境工程] O644[理学—物理化学]