H_(3)PO_(4)质子化改性的g-C_(3)N_(4)及其光催化产H_(2)O_(2)性能  

H_(3)PO_(4) Protonation-modified g-C_(3)N_(4) and Its Photocatalytic H_(2)O_(2) Production Properties

作　　者：郑娜 聂丽君 高宇航 薛坤坤 韩晓蓓 马跃宇 任丽蓉 苏王潮 石建惠 ZHENG Na;NIE Lijun;GAO Yuhang;XUE Kunkun;HAN Xiaobei;MA Yueyu;REN Lirong;SU Wangchao;SHI Jianhui(College of Environmental Science and Engineering,Taiyuan University of Technology,Taiyuan 030024,China)

机构地区：[1]太原理工大学环境与生态学院,太原030024

出　　处：《高等学校化学学报》2025年第4期92-102,共11页Chemical Journal of Chinese Universities

基　　金：国家自然科学基金(批准号:52100101)资助。

摘　　要：以三聚氰胺为前驱体,通过热缩聚法制备了块体石墨相氮化碳g-C_(3)N_(4)(BCN),并利用不同浓度的H_(3)PO_(4)对BCN进行水热处理,制备了质子化改性的g-C_(3)N_(4)(PBCNx),再经二甲基亚砜(DMSO)溶剂纯化,得到相应的PBCNx-D样品.通过X射线衍射(XRD)、傅里叶变换红外光谱(FTIR)、透射电子显微镜(TEM)、X射线光电子能谱(XPS)、元素分析(EA)和N2气吸附-脱附测试(BET)对样品进行了表征.结果表明,PBCNx-D不仅保留了g-C_(3)N_(4)的原始结构,而且具有松散的薄层结构、更大的比表面积及更多的氨基缺陷,这些特性提高了其光催化活性.瞬态光电流(TPC)、电化学阻抗(EIS)、光致发光光谱(PL)和紫外-可见漫反射光谱(UV-Vis DRS)分析结果表明,PBCNx-D的光生电子-空穴对复合率明显降低.BCN在质子化过程中形成了光响应较差的蜜勒胺分子,经DMSO溶剂纯化后,PBCNx-D的光电化学性能得到进一步提升.在光催化产H_(2)O_(2)实验中,PBCN10-D表现出最佳的光催化活性,光照5 h,H_(2)O_(2)产率为0.502 mmol/L,为初始BCN的7.17倍.In this study,bulk graphite phase carbon nitride g-C_(3)N_(4)(BCN)was prepared by using melamine as the precursor,BCN was hydrothermally treated with different concentrations of H_(3)PO_(4),to prepare protonated modified g-C_(3)N_(4)(PBCNx),and then PBCNx was purified by DMSO solvent to obtain the corresponding PBCNx-D sample.The structural morphology of the sample was characterized by X-ray diffraction(XRD),Fourier transform infrared spectroscopy(FTIR),transmission electron microscope(TEM),and X-ray photoelectron spectroscopy(XPS).The results prove that PBCNx-D not only retains the original structure of g-C_(3)N_(4),but also has a thin layer structure,larger surface area and more amino defects,and these properties enhance its photocatalytic activity.The analysis of transient photocurrent(TPC),electrochemical impedance(EIS),photoluminescence spectrum(PL)and UV-visible diffuse reflection spectrum(UV-Vis DRS)show that the electron-hole recombination of PBCNx-D is significantly reduced.It is worth noting that BCN forms poorly photoresponsive melem molecules during the protonation process.After purification with DMSO solvent,the photoelectrochemical properties of PBCNx-D are further improved.In the experiment of photocatalytic production of H_(2)O_(2),PBCN 10-D shows the best photocatalytic activity,with a H_(2)O_(2)yield of 0.502 mmol/L after 5 h of light irradiation,which is 7.17 times than that of the initial BCN.

关 键 词：质子化石墨相氮化碳 蜜勒胺 可见光 光催化产过氧化氢 

分 类 号：O643.36[理学—物理化学] O644.1[理学—化学]