水热反应前驱液pH对钨酸铋形貌结构及光催化性能调控  

Mechanism of morphology regulation and photocatalytic performance of bismuth tungstate by precursor pH in hydrothermal reactions

作　　者：刘婷婷 曹利兵 吴颜 闫梦鸽 杨帆宇 武峥 LIU Tingting;CAO Libing;WU Yan;YAN Mengge;YANG Fanyu;WU Zheng(School of Environmental and Chemical Engineering,Xi’an Polytechnic University,Xi’an 710048,China;Key Laboratory of Northwest Water Resources,Environment and Ecology,MOE,Xi’an University of Architecture and Technology,Xi’an 710055,China;Handan Municipal Bureau of Ecology and Environment,Handan 056000,China)

机构地区：[1]西安工程大学环境与化学工程学院,西安710048 [2]西安建筑科技大学西北水资源与环境生态教育部重点实验室,西安710055 [3]邯郸市生态环境局,邯郸056000

出　　处：《工程科学学报》2025年第4期958-969,共12页Chinese Journal of Engineering

基　　金：中国博士后科学基金资助项目(2023MD734204);陕西省教育厅自然科学专项研究计划资助项目(23JK0458);西安工程大学博士科研启动项目(310/107020512);陕西省重点产业创新链(群)项目(2022ZDLSF06-05);西北水资源与环境生态教育部重点实验室开放基金资助项目(2022SZY02)。

摘　　要：氟伐他汀作为常用的降血脂药物,常随人体排泄物排入水体.环境水体中的氟伐他汀很难被自然光所降解,长期累积会对环境构成一定的威胁.本研究采用钨酸铋(Bi_(2)WO_(6))可见光催化降解氟伐他汀,研究不同水热反应前驱液pH制备Bi_(2)WO_(6)的形貌结构及光电性能变化规律,结合活性自由基及中间产物解析揭示氟伐他汀降解机理.结果表明,前驱液pH由酸性转向中性时Bi_(2)WO_(6)晶体发育过程被破坏引起纳米片堆叠,前驱液pH为碱性时形成无序的八面体物相高聚体.随着pH升高,Bi_(2)WO_(6)的比表面积和孔径逐渐减小.当pH值为0.5时,Bi_(2)WO_(6)呈现有序的三维纳米花球结构,具有最佳光催化性能,光照120 min后氟伐他汀降解率达69.84%.经过四轮循环实验后,催化剂性能仍较为稳定.电化学实验结果表明,当前驱液pH值为0.5时,Bi_(2)WO_(6)具有最佳的光生电子-空穴(e^(-)-h^(+))分离性能,进而促进活性自由基高效产生.自由基实验结果表明,在降解过程中h^(+)发挥主要的氧化作用,·OH和·O_(2)^(-)起辅助作用.Bi_(2)WO_(6)降解氟伐他汀的机理是以h^(+)为主,·OH和·O_(2)^(-)为辅,联合攻击氟伐他汀分子的C-C键,形成小分子环状有机物、直链有机物和羟基化衍生物,进而将其矿化为CO_(2)和H_(2)O.Fluvastatin,a widely used lipid-lowering drug,is frequently released into water bodies via human excreta.Due to its resistance to natural light degradation,its prolonged accumulation in the environment may pose significant ecological risks.Semiconductor photocatalysis has gained increasing attention as an eco-friendly and versatile method for removing refractory pollutants.Among various photocatalysts,bismuth tungstate(Bi_(2)WO_(6))has emerged as a promising photocatalyst due to its strong visible-light response and high chemical stability.However,its application remains limited by its energy band structure,low separation efficiency of photogenerated carriers,and small specific surface area.In this study,Bi_(2)WO_(6) was utilized for the visible-light driven photocatalytic degradation of fluvastatin.The research investigates the influence of precursor pH during hydrothermal synthesis on the morphological structure and photoelectric properties of Bi_(2)WO_(6).Additionally,reactive radicals and intermediates analyses were conducted to elucidate the degradation mechanism of fluvastatin.The morphology,crystal phase,optical absorption performance,specific surface area,electrochemical performance,and carrier separation ability of the synthesized Bi_(2)WO_(6) photocatalyst were characterized using an electrochemical workstation and steady-state fluorescence spectroscopy.Its performance and stability were evaluated through degradation and cyclic experiments,and the effects of different pH conditions on photocatalytic efficiency were also examined.Additionally,active species analysis and intermediate product identification were employed to elucidate the degradation mechanism of fluvastatin.The results indicate that as the precursor pH shifts from acidic to neutral,the crystal growth of Bi_(2)WO_(6) is disrupted,leading to the stacking of nanosheets.Under alkaline conditions,disordered octahedral phase polymers are formed.The optimal precursor pH was found to be 0.5,yielding an ordered,three-dimensional nanoflower morpholo

关 键 词：钨酸铋 氟伐他汀 水热反应 前驱液pH 光催化性能 

分 类 号：X52[环境科学与工程—环境工程]