Cu/Al催化剂的制备及其在环丙沙星降解反应中的应用  

Preparation of Cu/Al heterogeneous Fenton-like catalyst and its application in ciprofloxacin degradation reaction

作　　者：李章良 张国鑫 张明静 吕源财[4] LI Zhangliang;ZHANG Guoxin;ZHANG Mingjing;LYU Yuancai(College of Environmental and Biological Engineering,Putian University,Putian 351100,China;Fujian Provincial Key Laboratory of Ecology-Toxicological Effects&Control for Emerging Contaminants,Putian 351100,China;Key Laboratory of Ecological Environment and Information Atlas,Fujian Provincial University,Putian 351100,China;College of Environment and Safety Engineering,Fuzhou University,Fuzhou 350108,China)

机构地区：[1]莆田学院环境与生物工程学院,莆田351100 [2]福建省新型污染物生态毒理效应与控制重点实验室,莆田351100 [3]生态环境及其信息图谱福建省高等学校重点实验室,莆田351100 [4]福州大学环境与安全工程学院,福州350108

出　　处：《环境工程学报》2022年第7期2135-2143,共9页Chinese Journal of Environmental Engineering

基　　金：国家自然科学基金资助项目(51908132);福建省自然科学基金资助项目(2020J01912);福建省大学生创新创业训练计划项目(S202111498015)。

摘　　要：为解决传统Fenton法在水体通常的酸碱(pH>6.0)条件下活性低的问题,采用水热合成法制备了掺杂Al的非均相铜基类芬顿催化剂,通过X射线衍射(XRD)、扫描电子显微镜(SEM)、X射线光电子能谱(XPS)及比表面与孔隙度分析(BET)等技术对其结构和形貌进行了表征;以20 mg·L^(-1)的环丙沙星(CIP)为目标污染物,研究了不同催化剂的非均相铜基类芬顿反应体系对CIP的降解效果及H_(2)O_(2)消耗量和·OH产生量的影响;探讨了Cu/Al-180催化剂投加量、H_(2)O_(2)投加量、初始pH 3个因素对Cu/Al-180催化剂的非均相类芬顿催化降解性能的影响;考察了催化剂的循环使用活性及稳定性。结果表明:不同温度下合成的Cu/Al催化剂主要组分是以CuO和少量Al_(2)O_(3)组成的介孔材料;Cu/Al-180催化剂具有较好的结晶度及均匀的颗粒状表面形貌,且对CIP具有最高的催化活性;在Cu/Al-180催化剂投加量为3.0 g·L^(-1)、H_(2)O_(2)投加量为149.55 mmol·L^(-1)、pH为5.0条件下,反应时间120 min时CIP降解率为93.3%;Cu/Al-180催化剂催化H_(2)O_(2)的pH范围明显拓展,在弱酸性和中性条件下表现出优良的催化性能;合成的Cu/Al-180催化剂经过5次连续循环使用后对CIP降解率可达64.2%,表明该催化剂具有较高的催化活性,且金属离子溶出量较少。To address the problem of low activity for traditional Fenton method in water under normal acidbase(pH>6.0)conditions,the heterogeneous copper based Fenton-like catalysts doped with Al were prepared by hydrothermal synthetic method.The structure and morphology were characterized by XRD,SEM,XPS and BET.With 20 mg·L^(-1)ciprofloxacin(CIP)as the target pollutant,the effects of heterogeneous copper based Fenton-like reaction systems with different catalysts on CIP degradation,H_(2)O_(2)consumption and·OH production were studied.The effects of catalyst dosages,H_(2)O_(2)dosages and initial pH on CIP degradation with Cu/Al-180 catalyst were discussed,as well as the recycling activities and stability of Cu/Al-180 catalyst.The results showed that the Cu/Al catalysts synthesized at different temperatures were the mesoporous material with CuO and a small amount of Al_(2)O_(3),of which Cu/Al-180 catalyst had good crystallinity and uniform granular surface morphology,and showed the highest catalytic activity for CIP.Under the reaction conditions of 3.0 g·L^(-1)catalyst dose,149.55 mol·L^(-1)H_(2)O_(2)dose and pH=5.0,CIP degradation rate could reach 93.3%within 120min.The Cu/Al-180/H_(2)O_(2)system widened the pH range,which resulted in superior organics removal even at mildacidic to medium pHs.CIP degradation rate maintained 64.2%even after five consecutive cycles,which indicates that Cu/Al-180 catalyst had a high catalytic activity and low copper ion release.

关 键 词：催化 非均相类芬顿法 Cu/Al催化剂 环丙沙星(CIP) 降解 

分 类 号：X703.1[环境科学与工程—环境工程]