Cu-Fe_(3)O_(4)/CDQ磁性仿酶催化剂的制备及性能研究  

Preparation and performance study of magnetic enzyme imitation catalyst of Cu-Fe_(3)O_(4)/CDQ

作　　者：缪光硕 李文兵 罗俊锋 吴伟浩 郭璇 孟瑶 周云辉 吴祖杰 李享成 MIAO Guangshuo;LI Wenbing;LUO Junfeng;WU Weihao;GUO Xuan;MENG Yao;ZHOU Yunhui;WU Zujie;LI Xiangcheng(School of Chemistry and Chemical Engineering,Wuhan University of Science and Technology,Wuhan 430081;State Key Laboratory of Coking Coal Resources Green Exploitation,Pingdingshan 467000;State Key Laboratory of Refractories and Metallurgy,Wuhan 430081)

机构地区：[1]武汉科技大学化学与化工学院,武汉430081 [2]炼焦煤资源绿色开发全国重点实验室,平顶山467000 [3]省部共建耐火材料与冶金国家重点实验室,武汉430081

出　　处：《环境科学学报》2024年第8期239-249,共11页Acta Scientiae Circumstantiae

基　　金：国家自然科学基金(No.52304410,51972242);湖北省自然科学基金创新群体项目(No.2020CFA038);炼焦煤资源绿色开发全国重点实验室开放基金课题(No.41040220201308)。

摘　　要：采用共沉淀法、浸渍法和煅烧法合成了Cu-Fe_(3)O_(4)/CDQ磁性非均相仿酶催化剂,并利用SEM、BET、FTIR、XRD、VSM、XPS等对合成催化剂进行了表征.同时,系统考察了该催化剂在不同体系以及不同变量(如pH、H2O2投加量和Cu-Fe_(3)O_(4)负载量等因素)对其降解苯酚性能的影响,并探究了其降解机理.结果表明,Cu-Fe_(3)O_(4)/CDQ材料具有介孔结构,Cu-Fe_(3)O_(4)纳米颗粒以球形颗粒的形式均匀分布在介孔改性焦炭上,其平均粒径为46.63 nm.Cu-Fe_(3)O_(4)/CDQ复合材料在pH=4~12范围处理含酚废水过程中具有较高的降解性能且表现出良好的稳定性和可重复使用性能.120 min内,在1 g·L^(-1)Cu-Fe_(3)O_(4)/CDQ、0.5 mL H2O2、Cu-Fe_(3)O_(4)负载量为40%、pH为10条件下,苯酚去除率达98.5%.铜离子和铁离子加速了Cu-Fe_(3)O_(4)/CDQ反应体系中·OH产生速率,促进了苯酚的降解.In this study,magnetic Cu-Fe_(3)O_(4)/modified coke dry quenching(Cu-Fe_(3)O_(4)/CDQ)composites were prepared by three steps of coprecipitation,dipping and calcination as a heterogeneous catalyst to degrade phenol.The morphological and structural properties of Cu-Fe_(3)O_(4)/CDQ were approved by scanning electron microscopy(SEM),energy dispersive X-ray(EDS),Bruneau Emmett Teller(BET),Fourier transform infrared spectroscopy(FTIR),X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),and vibrating sample magnetometry(VSM)techniques.The process and mechanism of heterogeneous catalyst synergistic catalytic degradation of phenol in Cu-Fe_(3)O_(4)/CDQ system were extensively evaluated.Results indicated that Cu-Fe_(3)O_(4)/CDQ possessed a mesoporous structure and Cu-Fe_(3)O_(4) nanoparticles in the form of spherical particles were uniformly distributed on mesoporous carbon through modified coke dry quenching for more unsaturated groups.The average particle size of Cu-Fe_(3)O_(4)/CDQ was 46.63 nm.The addition of Cu-Fe_(3)O_(4) achieved a high removal efficiency of phenol in a wide pH range of 4~12.Within 120 min,the phenol removal efficiency reached 98.5%by using 1.0 g·L^(-1) Cu-Fe_(3)O_(4)/CDQ,0.5 mL H2O2,and 40%capacity of Cu-Fe_(3)O_(4) at a pH of 10.The stability and reusability performance of Cu-Fe_(3)O_(4)/CDQ composites were excellent in the treatment process of phenolic wastewater.The synergistic effect of copper ions and iron ions accelerated the circulation of Fe(II)/Fe(III)and Cu(I)/Cu(II),which improved the electron transfer on the catalyst surface and increased the·OH free radical generation rate.

关 键 词：改性焦炭 Cu-Fe_(3)O_(4)/CDQ 降解 磁性 苯酚 

分 类 号：X703[环境科学与工程—环境工程]