苗志全 黄文璇 王拓 宋昀茜 袁国兴 吴凯 程立坤 赵纯

摘 要：以天然棉花為前驱物，通过直接一步热解法制备了新型碳纤维气凝胶（CFA）阴极，用于电化学臭氧技术（E-O3-CFA），通过SEM、BET、XPS等方法对CFA进行成分和结构分析，系统地研究了E-O3-CFA体系对水中布洛芬（IBP）的去除情况，考察了阴极材料、臭氧浓度、电流强度和初始pH值等因素的影响，分析该体系去除IBP的途径和机理，并对能耗进行计算。结果表明，CFA是一种多孔互联的三维网状结构，孔隙发达，比表面积高且表面存在丰富的含氧官能团，在电流强度为300 mA、O3浓度为16 mg/L、未调节初始pH值的条件下，E-O3-CFA体系对水中IBP的去除率高达97.96%，高于使用其他阴极材料的电化学臭氧体系（不锈钢阴极83.11%、活性炭纤维阴极94.78%、石墨阴极89.05%），CFA阴极的使用进一步降低了电化学臭氧体系的单位能耗（SEC=2.49 kW·h/gTOC），该体系主要通过以羟基自由基（·OH）为主的自由基路径氧化降解有机物。

关键词：臭氧;电化学;碳气凝胶阴极;布洛芬

中图分类号：X522;TU991.27   文献标志码：A   文章编号：2096-6717（2020）04-0176-09

收稿日期：2020-03-01

基金项目：国家自然科学基金（51308563）;中央高校基本科研业务费（2019CDXYCH0027）;重庆自然科学基金（cstc2019jcyjmsxmX0463）

作者简介：苗志全（1994- ），主要从事水处理高级氧化技术研究，E-mail：1131689604@qq.com。

赵纯（通信作者），副教授，博士生导师，E-mail：pureson@163.com。

Received：2020-03-01

Foundation items：National Natural Science Foundation of China （No. 51308563）; The Fundamental Research Funds for the Central Universities of China （No. 2019CDXYCH0027）; Chongqing Natural Science Foundation Project （No. cstc2019jcyjmsxmX0463）

Author brief：MIAO Zhiquan （1994- ）， main research interest： advanced oxidation technology for water treatment， E-mail： 1131689604@qq.com.

ZHAO Chun （corresponding author）， associate professor， doctorial supervisor， E-mail： pureson@163.com.

Removal of ibuprofen by electrolysis-ozone system with carbon fiber aerogel cathode

MIAO Zhiquan1a，1b， HUANG Wenxuan1b， WANG Tuo1a，1b， SONG Yunqian1a，1b， YUAN Guoxing2， WU Kai3， CHENG Likun3， ZHAO Chun1a，1b

（1a. State Key Laboratory of Coal Mine Disaster Dynamics and Control; 1b. Key Laboratory of the Three Gorges Reservoir Regions Eco-Environment， Ministry of Education， Chongqing University， Chongqing 400044， P. R. China; 2. Ningbo Chaochun Intelligent Technology Co. Ltd.， Ningbo 315100， Zhejiang， P. R. China; 3. Shanghai Qiyi Technology Co. Ltd.， Shanghai 200436， P. R. China）

Abstract： A novel carbon fiber aerogel was prepared by one-step direct pyrolysis method using natural cotton as a precursor， and the electrolysis-ozone technology using CFA cathode （E-O3-CFA） was established. The composition and structure of CFA were analyzed by SEM， BET and XPS. The removal of IBP and the main operational parameters （e.g.， cathode materials、current intensity、ozone concentration and pH） were evaluated systematically. The pathway and mechanism of IBP removal were also investigated， and the energy consumption was calculated. The results showed that CFA is a porous interconnected three-dimensional network structure with developed pores， high specific surface area and abundant oxygen-containing functional groups on the surface. The removal rate of IBP by E-O3-CFA process was 97.96% at ozone concentration of 16mg/L， current intensity of 300 mA， and without adjusting the initial pH. It was higher than the electrolysis-ozone technology with other cathode （steel cathode 83.11%、activated carbon fiber cathode 94.78%、graphite cathode 89.05%）. The IBP was mainly removed by the free radical oxidation pathway by ·OH. Moreover， the specific energy consumption （SEC=2.49 kW·h/gTOC） of electrolysis-ozone technology for TOC removal was furtherly reduced by using CFA cathode.

Keywords：ozone; electrolysis; carbon fiber aerogels; ibuprofen

布洛芬（IBP）作为一种镇痛类药物，被广泛用于治疗各种炎症性疾病。目前，全球每年产量已经超过千吨，并且这一数量正在逐年攀升。人类长期接触此种药物，会引起消化道感染并且削弱人体的免疫能力[1]，同时，IBP进入自然水体也会造成水生动物遗传性和全身性损害，并影响脊椎动物和无脊椎动物的性类固醇激素[2]。……