[关键词]
[摘要]
针对非均相光芬顿中两相传质阻力导致催化性能较低的缺陷,采用水热法制备了α-Fe2O3{110}/{113}晶面不同暴露比例的催化剂。采用X射线衍射分析(XRD)、透射电子显微镜(TEM/HRTEM)、傅里叶变换红外光谱(FTIR)以及紫外可见固体漫反射(UV-vis DRS)对催化剂进行表征分析,分别考察了H2O2浓度、催化剂投加量、甲基橙初始质量浓度以及初始pH对其催化降解甲基橙的影响,结果表明:FeCl3·6H2O浓度为33 mmol/L,摩尔比FeCl3·6H2O∶NaH2PO4∶NaF为1∶1∶15,180℃反应24 h所得α-Fe2O3催化性能最佳,在H2O2浓度为20 mmol/L,催化剂投加量为200 mg/L,甲基橙初始质量浓度为40 mg/L以及初始pH=5的条件下,对甲基橙的催化降解效果最佳,反应60 min去除率达97.83%;重复试验表明催化剂稳定性较好;H2O2消耗分析及自由基捕获实验结果表明,羟基自由基和光生空穴发挥关键催化降解作用,超氧自由基作用较小。
[Key word]
[Abstract]
To address the defect of low catalytic performance due to the two-phase mass transfer resistance in heterogeneous photo-Fenton, a hydrothermal method was used to prepare catalysts α-Fe2O3 that exposed different ratios of crystal plane {110}/{113}. α-Fe2O3 was characterized by XRD, TEM/HRTEM, FTIR and UV-vis DRS. The effects of H2O2 concentration, catalyst dosage, initial concentration of methyl orange and initial pH on α-Fe2O3 on methyl orange catalytic degradation were investigated. The results showed that the α-Fe2O3 achieved the best catalytic performance when the concentration of precursor FeCl3·6H2O was 33 mmol/L, the dosage ratio of FeCl3:6H2O:NaH2PO4:NaF was 1:1:15, and the reaction temperature was 180℃. Moreover, at the H2O2 dosage of 20 mmol/L, catalyst dosage of 200 mg/L, initial methyl orange concentration of 40 mg/L and initial pH of 5, the removal of methyl orange was the best, reaching 97.83% in 60 min. The catalyst exhibited good stability after consecutive degradation cycles. The H2O2 consumption analysis and free radical trapping experiment results showed that hydroxyl radicals and photo-generated holes played a key role in the catalytic degradation process, while superoxide radicals had less effect.
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[基金项目]
国家重点研发计划资助项目(2019YFD1100101-06)。