Fe3O4@β-CD nanocomposite as heterogeneous Fenton-like catalyst for enhanced degradation of 4-chlorophenol (4-CP)

催化作用 化学 氯苯 激进的 降级(电信) 纳米复合材料 浸出(土壤学) 动力学 核化学 反应速率常数 无机化学 化学工程 有机化学 工程类 土壤水分 土壤科学 物理 电信 量子力学 计算机科学 环境科学
作者
Manlin Wang,Guodong Fang,Peng Liu,Dongmei Zhou,Chen Ma,Dongju Zhang,Jinhua Zhan
出处
期刊:Applied Catalysis B-environmental [Elsevier BV]
卷期号:188: 113-122 被引量:282
标识
DOI:10.1016/j.apcatb.2016.01.071
摘要

The magnetic Fe3O4@β-cyclodextrin (β-CD) nanocomposites were fabricated via Fe ions and β-CD in one pot and characterized as a heterogeneous Fenton-like catalyst that may be used for the degradation of 4-chlorophenol (4-CP). The catalytic capacity of Fe3O4@β-CD was evaluated on the basis of various parameters, including pH, H2O2 concentration and catalyst loading, with regards to the pseudo-first-order kinetics of 4-CP degradation. In addition, iron leaching, the effect of radical scavengers and reusability of the Fe3O4@β-CD nanocomposite were also studied. The results showed that Fe3O4@β-CD exhibited a higher catalytic ability than that Fe3O4 toward 4-CP degradation, the observed rate constants (kobs) were 0.0373 min−1 for Fe3O4@β-CD, and 0.0162 min−1 for Fe3O4, which may be ascribed to the construction of a ternary complex (Fe2+–β-CD–pollutant) that allowed the produced hydroxyl radicals (·OH) to directly attack the contaminant and simultaneously enhanced the solubility of the organic pollutant. Fe3O4@β-CD also exhibited an enhancement effect for chlorobenzene (CB) degradation with the kobs of 0.0392 min−1 (kobs = 0.0099 min−1 for Fe3O4), which may be due to a synergistic effect in the Fe3O4@β-CD composite. Furthermore, Fe3O4@β-CD has an excellent catalytic activity, stable mechanical strength and adequate reusability. A possible reaction pathway of 4-CP degradation dominated by ·OH was proposed according to analyses of the degradation intermediates and chloride ions. The host-guest interaction between β-CD and 4-CP were examined with density functional theory (DFT) calculations, expounding the unicity of degraded intermediate owing to the specific spatial selectivity of β-CD. The findings of this study provide a novel material used in the Fenton-like process for the degradation of contaminants.
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