以三聚氰胺(Melamine)为原料,在高温条件下采用热缩合反应合成了石墨型氮化碳(g-C3N4)光催化剂.通过X-射线衍射(XRD)、扫描电镜(SEM)、紫外-可见漫反射光谱(UV-Vis DRS)、衰减全反射红外光谱(ATR-IR)等技术对其物理结构及性质进行了表征,结果表明实验制备的g-C3N4为片层状结构,比表面积为15.34 m~2·g^-1.在可见光(λ〉420 nm)照射下,用g-C3N4降解有机小分子污染物2,4-二氯苯酚(2,4-Dichlorophenol,2,4-DCP),该过程反应符合一级动力学,反应速率常数为0.0113 min^-1,以0.67 g·L^-1的用量反应250 min后2,4-DCP矿化率达到60%;2,4-DCP在弱酸性条件下(p H=5.4)的降解效率最高;通过捕获实验及电子自旋共振(ESR)实验表明,超氧自由基(O·-2)是g-C3N4光催化降解2,4-DCP过程中的主要活性物种.2,4-DCP的降解路径主要涉及脱氯、苯环开环和碳链断裂等反应历程.
Graphite carbon nitride (g-C3N4) photocatalyst was synthesized via thermal condensation at high temperatures using melamine as a starting material. The structure and properties of the catalyst was characterized by scanning electron microscopy (SEM),X-ray diffraction (XRD),UV-Vis diffuse reflectance spectroscopy (UV-Vis DRS), and attenuated total reflection infrared spectroscopy (ATR-IR).The results indicate that the as-synthesized g-C3N4 had a layered structure with a specific surface area of 15.34 m2·g-1 and possed strong visible light absorption capacity. Photocatalytic degradation of 2,4-dichlorophenol (2,4-DCP) using g-C3N4 under visible light irradiation (λ〉420 nm) corresponds to the first order kinetics with a reaction rate constant of 0.0113 min-1.After 250 min,the mineralization rate of 2,4-DCP in the presence of 0.67 g·L-1g-C3N4 reached 60%. The degradation efficiency of 2,4-DCP was highly enhanced in weak acid. Trapping experiments and electron spin resonance (ESR) experiments show that superoxide radical (O2·-) was the main active species in the photocatalytic degradation of 2,4-DCP.The main degradation pathways of 2,4-DCP include dechlorination,aromatic ring opening and carbon chain rupture.