A Mechanistic Understanding of Hydrogen Peroxide Decomposition by Vanadium Minerals for Diethyl Phthalate Degradation
A Mechanistic Understanding of Hydrogen Peroxide Decomposition by Vanadium Minerals for Diethyl Phthalate Degradation
复制标题
钒矿物分解过氧化氢降解邻苯二甲酸二乙酯的机理理解。
DOI：
10.1021/acs.est.7b05303
复制
发表时间：
2018-02-20
影响因子：
11.4
通讯作者：
Zhou, Dongmei
中科院分区：
文献类型：
--
作者：
Fang, Guodong;Deng, Yamei;Zhou, Dongmei
在原位化学氧化（ISCO）处理中，天然矿物与H2 O2的相互作用影响污染场地的修复效率。然而，钒（V）矿物和H2 O2之间的相互作用很少被探索。在这项研究中，H2 O2分解的各种含钒矿物，包括V（III），V（IV），和V（V）的氧化物进行了检查，羟基自由基（（OH）-O-中心点）产生的污染物降解的机制进行了研究。钒酸盐矿物能有效地催化H2 O2分解产生（OH）-O-中心点，在较宽pH范围的水溶液和土壤中降解邻苯二甲酸二乙酯（DEP）。电子顺磁共振（EPR）、X射线光电子能谱（XPS）、X射线衍射（XRD）和自由基猝灭研究表明，（OH）-O-中心点是由V（III）/V（IV）通过单电子转移途径在V2 O3和VO 2颗粒表面生成的，而氧空位（OV）则是V_2O_5颗粒表面形成（OH）-O中心点的主要原因。该研究为钒矿物与H2 O2在H2 O2基ISCO反应中的作用机理提供了新的认识。
The interaction of naturally occurring minerals with H2O2 affects the remediation efficiency of polluted sites in in situ chemical oxidation (ISCO) treatments. However, interactions between vanadium(V) minerals and H2O2 have rarely been explored. In this study, H2O2 decomposition by various vanadium-containing minerals including V(III), V(IV), and V(V) oxides was examined, and the mechanism of hydroxyl radical ((OH)-O-center dot) generation for contaminant degradation was studied. Vanadium minerals were found to catalyze H2O2 decomposition efficiently to produce (OH)-O-center dot for diethyl phthalate (DEP) degradation in both aqueous solutions with a wide pH range and in soil slurry. Electron paramagnetic resonance (EPR), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD) analyses, and free radical quenching studies suggested that (OH)-O-center dot was produced via single electron transfer from V(III)/V(IV) to H2O2 followed a Fenton-like pathway on the surface of V2O3 and VO2 particles, whereas the oxygen vacancy (OV) was mainly responsible for (OH)-O-center dot formation on the surface of V2O5 particles. This study provides new insight into the mechanism of interactions between vanadium minerals and H2O2 during H2O2-based ISCO.