BaSnO3钙钛矿光催化降解邻苯二甲酸二乙酯的机理研究  

Insights into photocatalytic degradation of diethyl phthalate over BaSnO3 perovskite

作　　者：叶权运 李想 马晓蕊 李沛然 柳王荣 贺德春 佘磊 YE Quan-yun;LI Xiang;MA Xiao-rui;LI Pei-ran;LIU Wang-rong;HE De-chun;SHE Lei(South China Institute of Environmental Sciences,Ministry of Ecology and Environment,Guangzhou 510530,China)

机构地区：[1]生态环境部华南环境科学研究所,广东广州510530

出　　处：《中国环境科学》2023年第3期1208-1215,共8页China Environmental Science

基　　金：科技兴蒙项目(2020-科技兴蒙-国创中心-14);中央级公益性科研院所基本科研业务费专项资金资助项目(PM-zx703-202204-117)。

摘　　要：以邻苯二甲酸二乙酯(DEP)为目标污染物,研究了BaSnO3锡酸盐钙钛矿在模拟太阳光条件下对其光催化降解的潜力.现代谱学表征结果表明BaSnO3钙钛矿具有丰富的氧空位、结构缺陷和优异的光催化活性,在500W氙灯照射下,120min内能降解91.8%的DEP(10mg/L),降解过程符合准一级动力学,且BaSnO3钙钛矿在pH值3.0~9.0范围内均保持良好的催化性能.光生空穴(h^(+))、超氧自由基(O_(2)·^(-))和羟基自由基(·OH)均参与了光降解反应,其中O_(2)·^(-)起最主要的降解作用.通过密度泛函理论计算(DFT)对DEP的降解路径和机理进行研究,发现活性氧基团(包括O_(2)·^(-)和·OH)对DEP苯环羟基化和脂肪链断裂起重要贡献.The photocatalytic degradation potential of BaSnO3stannate perovskite was investigated under simulated sunlight, where diethyl phthalate(DEP) was selected as the probe pollutants.The results of modern spectral analysis showed that BaSnO3perovskite with abundant oxygen vacancies, structural defects, and excellent photocatalytic activity could effectively degrade 91.8% of DEP through pseudo-first-order reaction kinetics, and it also remained good degradation efficiency in the pH from 3.0 to 9.0.The photogenerated holes(h+), superoxide(O_(2)·^(-)), and hydroxyl radicals(·OH) participated in the photo-degradation, among which O_(2)·^(-)played the most important role.Furthermore, the degradation mechanism was explored using density functional theory(DFT)calculations, proving that the reactive oxygen species(including O_(2)·^(-)and·OH) were responsible for the hydroxylation of benzene ring and the breaking of the aliphatic chain, while h+was prone to break the aliphatic chain.

关 键 词：锡酸盐 钙钛矿 光催化 邻苯二甲酸二乙酯 密度泛函理论 

分 类 号：X703[环境科学与工程—环境工程]