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Kinetics and mechanism for omethoate degradation by catalytic ozonation with Fe(III)-loaded activated carbon in water

机译:负载Fe(III)的活性炭催化臭氧氧化氧化乐果酸盐的动力学和机理

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摘要

The kinetics and mechanism for degradation of omethoate (OMT) by catalytic ozonation with Fe(III)-loaded activated carbon (Fe@AC) were investigated in this study with focus on identification of degradation byproducts. The rate constants of OMT reacting with ozone and hydroxyl radical ((OH)-O-center dot) were determined to be 0.04 and 5.3 x 10(8) M-1 s(-1) at pH 7.5 and 20 degrees C, respectively. OMT was predominantly degraded by (OH)-O-center dot in the catalytic ozonation with Fe@AC. The high-molecular-weight degradation byproducts identified were O,O,O-trimethyl phosphoric ester (TMP), pyrrolidin-2-one, N-methyl-2-sulfanylacetamide, 2-(methylthio)acetamide, O,O,S-trimethylthiophosphate (STMP), and N-methyl-2-(methylthio) acetamide. Besides, low-molecular-weight organic acids and inorganic anions were also detected and quantified, including formic, acetic and oxalic acids as well as nitrate, sulfate and phosphate ions. In the catalytic ozonation, TMP and phosphate were two major P-containing byproducts resulting from OMT degradation. The toxicity of OMT solution gradually decreased during the catalytic ozonation, indicating that Fe@AC is a safe catalyst for OMT removal by ozone in water. (c) 2012 Elsevier Ltd. All rights reserved.
机译:在这项研究中,重点研究了降解副产物的鉴定,研究了负载Fe(III)的活性炭(Fe @ AC)催化臭氧氧化降解氧化乐果(OMT)的动力学和机理。确定OMT与臭氧和羟基自由基((OH)-O-中心点)反应的速率常数分别为pH 7.5和20摄氏度时为0.04和5.3 x 10(8)M-1 s(-1) 。 OMT在Fe @ AC催化臭氧氧化反应中主要被(OH)-O-中心点降解。鉴定出的高分子量降解副产物为O,O,O-三甲基磷酸酯(TMP),吡咯烷丁-2-酮,N-甲基-2-硫烷基乙酰胺,2-(甲硫基)乙酰胺,O,O,S-三甲基硫代磷酸酯(STMP)和N-甲基-2-(甲硫基)乙酰胺。此外,还检测并定量了低分子量有机酸和无机阴离子,包括甲酸,乙酸和草酸以及硝酸根,硫酸根和磷酸根离子。在催化臭氧化中,TMP和磷酸盐是OMT降解导致的两种主要的含P副产物。在催化臭氧氧化过程中,OMT溶液的毒性逐渐降低,表明Fe @ AC是水中臭氧去除OMT的安全催化剂。 (c)2012 Elsevier Ltd.保留所有权利。

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