李超,陈晓飞,岳欣,邢茜,牛建瑞,李再兴,田占伟,白晓松,赫彦利.钙钛矿型LaFexCu(1-xO3固相芬顿催化剂制备及其降解亚甲基蓝性能研究[J].分子催化编辑部,2021,35(6):503-517
钙钛矿型LaFexCu(1-xO3固相芬顿催化剂制备及其降解亚甲基蓝性能研究
Preparation of Perovskite LaFexCu(1-x)O3 Heterogeneous Fenton Catalyst and Its Degradation of Methylene Blue
投稿时间:2021-09-24  修订日期:2021-11-15
DOI:10.16084/j.issn1001-3555.2021.06.002
中文关键词:  钙钛矿催化剂  LaFexCu(1-xO3  固相芬顿  亚甲基蓝  共沉淀法
英文关键词:perovskite catalyst  LaFexCu(1-x) O3  heterogeneous fenton  methylene Blue  Co-precipitation method
基金项目:石家庄市科学技术研究与发展计划项目(211240043A,191240263A)
作者单位E-mail
李超 河北科技大学 环境科学与工程学院, 河北 石家庄 050018
河北省污染防治生物技术实验室, 河北 石家庄 050018 
 
陈晓飞 天俱时工程科技集团有限公司, 河北 石家庄 050011  
岳欣 河北科技大学 环境科学与工程学院, 河北 石家庄 050018
河北省污染防治生物技术实验室, 河北 石家庄 050018 
 
邢茜 天俱时工程科技集团有限公司, 河北 石家庄 050011  
牛建瑞 河北科技大学 环境科学与工程学院, 河北 石家庄 050018
河北省污染防治生物技术实验室, 河北 石家庄 050018 
 
李再兴 河北科技大学 环境科学与工程学院, 河北 石家庄 050018
河北省污染防治生物技术实验室, 河北 石家庄 050018 
li_zaixing@163.com 
田占伟 石家庄东华金龙化工有限公司, 河北 石家庄 052165  
白晓松 石家庄东华金龙化工有限公司, 河北 石家庄 052165  
赫彦利 石家庄东华金龙化工有限公司, 河北 石家庄 052165  
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中文摘要:
      采用共沉淀法制备系列钙钛矿型催化剂LaFexCu(1-xO3x=0.2,0.4,0.6,0.8),通过XRD、FT-IR、SEM、BET和XPS进行表征.以亚甲基蓝(Methylene Blue,MB)为模型污染物,将LaFexCu(1-xO3的催化性能与LaFeO3和LaCuO3进行比较,确定最佳掺杂比例.考察不同因素对催化反应的影响,确定最佳反应条件,并研究催化反应机理和催化剂的稳定性.结果表明:LaFexCu(1-xO3呈钙钛矿晶型结构,颗粒空间分布松散,孔道丰富,比表面积和平均孔径较大,从而有利于亚甲基蓝的催化降解.当x=0.6时,LaFe0.6Cu0.4O3具有最高的比表面积,同时催化活性最高.最佳条件:亚甲基蓝初始浓度为1000 mg·L-1,温度55℃、初始pH值为4、双氧水投加量2.5 mL·L-1、LaFe0.6Cu0.4O3投加量60 mg·L-1.在最佳条件下,亚甲基蓝在20 min内催化降解完全脱色,50 min内COD去除率和TOC去除率分别达到94.25%和84.34%.ESR测试表明亚甲基蓝降解是在羟基自由基(·OH)和超氧自由基(·HO2)共同作用下完成的.10次循环后脱色率、COD去除率和TOC去除率仍能分别达到90.27%、84.26%和80.29%,证明LaFe0.6Cu0.4O3是一种高效稳定的非均相催化剂.
英文摘要:
      A series of perovskite-type LaFexCu(1-x) O3(x=0.2, 0.4, 0.6, 0.8) catalysts were prepared by co-precipitation method. The catalysts were characterized by XRD, FT-IR, SEM, BET and XPS. The catalytic activity of LaFexCu(1-x) O3, LaFeO3 and LaCuO3 was compared by the degradation of Methylene Blue (MB), and the optimum doping ratio was determined. The influence of several factors on the reaction were studied to determine the optimum conditions, and the mechanism of reaction and the stability of catalyst were investigated. The results show that LaFexCu(1-x) O3 had a perovskite crystal structure, with loose particle spatial distribution, abundant pores, large specific surface area and average pore size, which was beneficial to the degradation of methylene blue. LaFe0.6Cu0.4O3 had the highest surface area and catalytic activity at x=0.6. Optimum conditions:initial concentration of methylene blue was 1000 mg·L-1, 55℃, initial pH value was 4, the dosage amount of hydrogen peroxide was 2.5 ml·L-1 and the dosage amount of catalyst is 60 mg·L-1. Under the optimal conditions, the methylene blue was completely decolorized by catalytic degradation within 20 minutes, and the COD removal rate and TOC removal rate reached 94.25% and 84.34% within 50 minutes, respectively. ESR showed that MB was degraded under the combined action of ·OH and ·HO2. After 10 cycles, the decolorization rate, COD removal rate and TOC removal rate can still reach 90.27%, 84.26% and 80.29%, respectively, which proved that LaFe0.6Cu0.4O3 was an efficient and stable heterogeneous catalyst.
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