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[纳米Fe3O4-H2O2体系类芬顿异相反应催化邻苯二酚氧化]

[Catalyzed oxidation of catechol by the heterogeneous Fenton-like reaction of nano-Fe3O4-H2O2 system].

作者信息

He Jie, Yang Xiao-fang, Zhang Wei-jun, Wang Dong-sheng

机构信息

State Key Laboratory of Environmental Aquatic Chemistry, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China.

出版信息

Huan Jing Ke Xue. 2013 May;34(5):1773-81.

Abstract

A Fenton-like system, consisting of magnetite (Fe3O4) and hydrogen peroxide (H2O2), was utilized to remove refractory organic pollutants using the hydroxyl radicals generated from the decomposition of H2O2. The characteristic of the catalyzed oxidation of catechol in a nano-Fe3O4-H2O2 Fenton-like system was studied. The catalytic activity of the synthesized nano-Fe3O4 was compared to that of the purchased micro-Fe3O4. The effect of initial H2O2 concentration on the oxidation of catechol was also studied. Results showed that the removal of catechol and total organic carbon and the decomposition of H2O2 were faster in the nano-Fe3O4-H2O2 system than in the purchased-Fe3O4-H2O2 system. The removal of catechol achieved nearly 100% in the former system. The catalyzed oxidation of catechol in nano-Fe3O4-H2O2 system followed pseudo-first-order kinetics. The decomposition of H2O2 could be fitted by third-order kinetics. The release of total iron was below 0.3 mg x L(-1), implying that the homogeneous Fenton reaction was not dominant. Therefore, surface reaction controlled heterogeneous Fenton-like reaction mechanism was deduced.

摘要

一种由磁铁矿(Fe3O4)和过氧化氢(H2O2)组成的类芬顿体系被用于利用H2O2分解产生的羟基自由基去除难降解有机污染物。研究了纳米Fe3O4-H2O2类芬顿体系中邻苯二酚催化氧化的特性。将合成的纳米Fe3O4的催化活性与购买的微米级Fe3O4的催化活性进行了比较。还研究了初始H2O2浓度对邻苯二酚氧化的影响。结果表明,纳米Fe3O4-H2O2体系中邻苯二酚和总有机碳的去除以及H2O2的分解比购买的Fe3O4-H2O2体系更快。在前一个体系中邻苯二酚的去除率接近100%。纳米Fe3O4-H2O2体系中邻苯二酚的催化氧化遵循准一级动力学。H2O2的分解可以用三级动力学拟合。总铁的释放量低于0.3 mg·L(-1),这意味着均相芬顿反应不占主导。因此,推导了表面反应控制的非均相类芬顿反应机理。

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