磷掺杂g-C_(3)N_(4)纳米片光催化降解盐酸四环素  

Photocatalytic degradation of tetracycline hydrochloride by phosphorus-doped g-C_(3)N_(4) nanosheets

作　　者：殷旭东 孙晓杰[1,2] 李德豪[3,4] 谢文玉 毛玉凤[3,4] 刘志森 刘正辉[3,4] YIN Xudong;SUN Xiaojie;LI Dehao;XIE Wenyu;MAO Yufeng;LIU Zhisen;LIU Zhenghui(Guangxi Key Laboratory of Environmental Pollution Control Theory and Technology,Guilin University of Technology,Guilin 541006,China;College of Environmental Science and Engineering,Guilin University of Technology,Guilin 541006,China;School of Environmental Science and Engineering,Guangdong University of Petrochemical Technology,Maoming 525000,China;Key Laboratory of Petrochemical Pollution Control of Guangdong Higher Education Institutes,Guangdong University of Petrochemical Technology,Maoming 525000,China)

机构地区：[1]桂林理工大学环境科学与工程学院,广西桂林541006 [2]桂林理工大学广西环境污染控制理论与技术重点实验室,广西桂林541006 [3]广东石油化工学院环境科学与工程学院,广东茂名525000 [4]广东石油化工学院广东高校石油化工污染控制重点实验室,广东茂名525000

出　　处：《桂林理工大学学报》2024年第3期502-510,共9页Journal of Guilin University of Technology

基　　金：国家自然科学基金项目(21777034,52070049);茂名市科技计划立项项目(2020545,2020KJZX032,2020KJZX033)。

摘　　要：针对无金属g-C_(3)N_(4)基光催化材料光激发载流子的快速复合限制了其光催化活性的问题,以双氰胺和羟基乙叉二膦酸(HEDP)为前驱体,结合形貌调控和磷掺杂两种改性方法,制备了不同磷(P)掺杂量的石墨相氮化碳(g-C_(3)N_(4))纳米片(PCNNS),对其形貌结构和光学性质进行了表征分析,并研究了降解盐酸四环素(TCH)的光催化性能和降解机理。结果表明:PCNNS-0.5降解速率最高,为块体g-C_(3)N_(4)(BCN)的2.52倍,降解动力学均符合伪一级反应动力学模型;·O^(-)_(2)和h^(+)是降解过程中的主要活性物种;经过4次循环实验,PCNNS-0.5仍具有较高的稳定性和良好的性能。PCNNS良好的光催化性能归因于P原子取代g-C_(3)N_(4)中碳原子所产生的良好的结构、光学和电子性质。Metal-free g-C_(3)N_(4) based photocatalytic materials are widely used for the degradation of antibioticwastewater due to their non-toxic and non-hazardous nature, stable chemical structure and low cost. However,the rapid compounding of their photoexcited carriers limit their photocatalytic activity. In this study, combiningmorphology modulation and phosphorus doping two modification methods, graphite-phase carbon nitride(g-C_(3)N_(4)) nanosheets(PCNNS) with different phosphorus(P) doping amounts are prepared using dicyandiamideand hydroxyethylidene diphosphonic acid(HEDP) as the precursors. The morphological structure and opticalproperties are characterized, and the photocatalytic performance and degradation mechanism of tetracyclinehydrochloride(TCH) are investigated. The results show that the degradation rate of PCNNS-0. 5 is the highest,which is 2. 52 times of that of bulk graphitic phase carbon nitride(BCN), and the degradation kinetics are allconsistent with a pseudo primary reaction kinetic model;·O^(-)_(2) and h^(+) are the main active species in the degradationprocess;after four cycles of experiments, PCNNS-0. 5 still has high stability and good performance. Thegood photocatalytic performance of PCNNS is attributed to the good structural, optical and electronic propertiesresulting from the substitution of phosphorus atoms for carbon atoms in g-C_(3)N_(4).

关 键 词：磷掺杂 石墨相氮化碳 盐酸四环素 光催化性能 机理 

分 类 号：TQ174[化学工程—陶瓷工业]