苯乙炔铜协同PMS光催化降解磺胺二甲嘧啶的机理研究  

Mechanism of synergistic photocatalytic degradation of sulfamethazine withcopper-phenylacetylide and peroxymonosulfate( PMS)

作　　者：林子力 张舸 刘国光[1] 张筱昱 王奕舜 刘德柱 牛梦洋 肖震钧 陈平[1] 吕文英[1] LIN Zili;ZHANG Ge;LIU Guoguang;ZHANG Xiaoyu;WANG Yishun;LIU Dezhu;NIU Mengyang;XIAO Zhenjun;CHEN Ping;LÜ Wenying(Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control,Guangdong-Hong Kong-Macao Joint Laboratory for Contaminants Exposure and Health,School of Environmental Science and Engineering,Guangdong University of Technology,Guangzhou 510006)

机构地区：[1]广东工业大学环境科学与工程学院,粤港澳污染物暴露与健康联合实验室,广东省环境催化与健康风险控制重点实验室,广州510006

出　　处：《环境科学学报》2024年第2期47-58,共12页Acta Scientiae Circumstantiae

基　　金：国家自然科学基金项目(No.22176042,22076029,21906029)。

摘　　要：基于过一硫酸盐(PMS)的高级氧化技术(SR-AOPs)在废水处理中引起广泛关注.本工作成功合成苯乙炔铜(PhC_(2)Cu)光催化剂并构建新型的PhC_(2)Cu/PMS体系,并进行可见光下降解磺胺二甲嘧啶(SMT)的机理研究.紫外-可见漫反射光谱、荧光发射光谱和光电化学测试表明PhC_(2)Cu具有良好的光电化学特性.PhC_(2)Cu光催化活化PMS可以产生多种活性物种,并且PMS捕获电子能提高PhC_(2)Cu界面电荷传输效率和光生载流子的分离效率,进而来提高PhC_(2)Cu/PMS体系的光催化性能.值得注意的是,PhC_(2)Cu/PMS体系在低功率蓝色LED灯下使SMT的降解率在30 min内高达97.65%,其反应速率分别是PhC_(2)Cu添加PMS(无光照)情况下的7.70倍和PhC_(2)Cu光照下(无添加PMS)的5.62倍.通过一系列环境影响因素(pH、离子、实际水体等)实验表明PhC_(2)Cu/PMS体系具有极大的实际应用潜力.循环实验表明,PhC_(2)Cu/PMS具有可靠的光催化稳定性和可循环使用性.此外,还揭示了PhC_(2)Cu活化PMS光催化降解SMT过程的电子转移途径.得益于PhC_(2)Cu极负的导带(CB)电位,该体系产生的丰富的光生电子有利于活化PMS及促进光催化过程中活性物种的生成.实验结果表明,超氧自由基(O_(2)^(·-))和单线态氧(^(1)O_(2))是SMT降解的主要活性物种.这项工作有助于为基于苯乙炔铜的新型光催化剂协同PMS增强有机污染物的降解提供理论指导和科学依据.Sulfate radical based advanced oxidation processes(SR-AOPs)have attracted much attention in the field of wastewater treatment due to their ability to produce reactive species by activating peroxonosulfate(PMS).In this work,we successfully synthesized copper-phenylacetylide(PhC_(2)Cu)photocatalyst and constructed a novel PhC_(2)Cu/PMS system to investigate the mechanism of photocatalytic degradation of sulfamethazine(SMT).Characterization techniques such as UV-vis diffuse reflectance,photoluminescence spectra and photoelectrochemical measurements were employed to evaluate the phtochatalytic properties of PhC_(2)Cu.These analyses revealed that the PhC_(2)Cu exhibits favorable photocatalytic activation of PMS,which could generate multiple reactive species and improve the charge transfer and the separation efficiency of photogenerated charges via PMS electron trapping.Notably,under low-power blue LED light,the degradation efficiency of SMT in PhC_(2)Cu/PMS system reached 97.65%within 30 min,and the constant rate is 7.70 times and 5.62 times higher than that of the PhC_(2)Cu without light and without PMS,respectively.In addition,various environmental factors(e.g.,pH value,ions,and actual water system,etc.)were investigated through a series of experiments,demonstrating the great potential of the PhC_(2)Cu/PMS for practical application.Cyclic experiments confirmed the reliable reliable photocatalytic stability and recyclability of the PhC_(2)Cu/PMS system.In addition,the electron transfer pathway for the photocatalytic degradation of SMT by PhC_(2)Cu-activated PMS was revealed.The highly negative conduction band(CB)potentials of PhC_(2)Cu facilitated the production of abundant photogenerated electrons,promoting the activation of PMS and the formation of reactive species during the photocatalysis process.The superoxide radical(O_(2)^(·-))and singlet oxygen(^(1)O_(2))were the main reactive species for SMT.This work provides theoretical guidance and scientific basis for a novel PhC_(2)Cu-based photocatalyst in conjunction

关 键 词：苯乙炔铜 过一硫酸盐 磺胺二甲嘧啶 光催化 降解机理 

分 类 号：X13[环境科学与工程—环境科学]