金属有机框架(MOFs)基电催化膜活化过硫酸盐降解磺胺甲噁唑  

Degradation of sulfamethoxazole by metal-organic framework(MOFs)-based electrocatalytic membrane activated by peroxymonosulfate

作　　者：张水珍 李墨华 李方[1,2] 陈泉源 刘艳彪[1,2] ZHANG Shuizhen;LI Mohua;LI Fang;CHEN Quanyuan;LIU Yanbiao(College of Environmental Science and Engineering,Donghua University,2999 North Renmin Road,Shanghai,201620,China;Shanghai Institute of Pollution Control and Ecological Security,Shanghai,200092,China)

机构地区：[1]东华大学环境科学与工程学院,上海201620 [2]上海污染控制与生态安全研究院,上海200092

出　　处：《环境化学》2023年第11期3779-3788,共10页Environmental Chemistry

基　　金：国家自然科学基金(52170068)资助。

摘　　要：基于过硫酸盐(peroxymonosulfate,PMS)活化的高级氧化技术在降解新污染物方面具有独特优势.本实验利用碳纳米管(carbon nanotubes,CNT)搭载Ni-ZIF-8,设计制备了CNT/Ni-ZIF-8纳米复合电催化膜,开展了活化过硫酸盐降解磺胺甲噁唑(sulfamethoxazole,SMX)的性能和机理研究.探究了制备条件与纳米复合膜理化性质间的构效关系,分析并优化了镍的掺杂量,考察了降解实验参数(如电压、流速和PMS用量等)对SMX降解动力学的影响.研究表明,Ni-ZIF-8均匀地负载在碳纳米管表面.在最佳条件时(镍掺杂量为20%、电压为-1.5 V、流速为1.5 mL·min^(-1)和PMS用量为1.5 mmol·L^(-1)),单次流模式下去除5 mg·L^(-1) SMX的效率为76.6%.电子顺磁共振谱和淬灭实验结果表明,·OH和^(1)O_(2)均参与到SMX的降解过程中.本研究为开发高效电催化膜催化材料提供了新的设计思路.Peroxymonosulfate(PMS)activation-based advanced oxidation technology has attracted wide attention toward the decontamination of emerging contaminants.In this study,carbon nanotubes(CNT)were used to host Ni-ZIF-8 to construct CNT/Ni-ZIF-8 electrocatalytic membranes.Their catalytic performance and mechanism for persulfate activation and degradation of sulfamethoxazole(SMX)were studied systematically.The correlation between preparation parameters and physicochemical properties of the catalytic membranes were investigated.The doping amount of nickel was analyzed and optimized.The effects of operational parameters(such as voltage,flow rate and PMS dosage)on the SMX degradation kinetics were identified.Results suggested that Ni-ZIF-8 nanoparticles were uniformly loaded onto the CNT surface.Under optimal conditions(e.g.,Ni doping of 20%,applied voltage of-1.5 V,flow rate of 1.5 mL·min^(-1) and PMS dosage of 1.5 mmol·L^(-1)),76.6%removal of 5 mg·L^(-1) SMX removal can be obtained under single-pass mode.Electron paramagnetic resonance(EPR)and radical quenching tests collectively suggested both·OH and ^(1)O_(2) were involved into the SMX degradation process.This study provides new insights on the development of high-performance electrocatalytic membranes for water treatment applications.

关 键 词：碳纳米管 金属有机框架 过硫酸盐 高级氧化 磺胺甲噁唑 

分 类 号：TQ426[化学工程] X703[环境科学与工程—环境工程]