高铁酸盐（VI）降解对乙酰氨基酚的反应动力学及氧化产物生成
Reaction kinetics and oxidation product formation in the degradation of acetaminophen by ferrate (VI).
作者信息
Wang Hongyu, Liu Yibing, Jiang Jia-Qian
机构信息
School of Civil Engineering and Architecture, Zhejiang University of Technology, Hangzhou 310014, People's Republic of China.
School of Civil Engineering and Architecture, Zhejiang University of Technology, Hangzhou 310014, People's Republic of China.
出版信息
Chemosphere. 2016 Jul;155:583-590. doi: 10.1016/j.chemosphere.2016.04.088. Epub 2016 May 4.
This paper investigates the degradation of acetaminophen (AAP) in aqueous solutions by ferrate (VI), aiming to propose the kinetics, pathways and the oxidation products' formation in the AAP degradation. A series of jar tests were undertaken over ferrate (VI) dosages (molar ratios of ferrate (VI):AAP, 5:1 to 25:1) and pH values (4-11). The effects of co-existing ions (0.2-5 mM) and humic acid (10-50 mg l(-1)) on the AAP removal were investigated. Ferrate (VI) can remove 99.6% AAP (from 1000 μg l(-1)) in 60 min under study conditions when majority of the AAP reduction occurred in the first 5 min. The treatment performance depended on the ferrate(VI) dosage, pH and the type and strength of co-existing ions and humic acid. Raising ferrate (VI) dosage with optimal pH 7 improved the AAP degradation. In the presence of humic acid, the AAP degradation by ferrate (VI) was promoted in a short period (<30 min) but then inhibited with increasing in humic acid contents. The presence of Al(3+), CO3(2-) and PO4(3-) ions declined but the existence of K(+), Na(+), Mg(2+) and Ca(2+) ions can improve the AAP removal. The catalytic function of Al(3+) on the decomposition of ferrate (VI) in aqueous solution was found. The kinetics of the reaction between ferrate (VI) and AAP was pseudo first-order for ferrete (VI) and pseudo second-order for AAP. The pseudo rate constant of ferrate (VI) with AAP was 1.4 × 10(-5) L(2) mg(-2) min(-1). Three oxidation products (OPs) were identified and the AAP degradation pathways were proposed.
本文研究了高铁酸盐（VI）对水溶液中对乙酰氨基酚（AAP）的降解作用，旨在提出AAP降解过程中的动力学、途径以及氧化产物的形成情况。针对高铁酸盐（VI）的剂量（高铁酸盐（VI）与AAP的摩尔比为5:1至25:1）和pH值（4 - 11）进行了一系列烧杯试验。研究了共存离子（0.2 - 5 mM）和腐殖酸（10 - 50 mg l⁻¹）对AAP去除效果的影响。在研究条件下，高铁酸盐（VI）在60分钟内可去除99.6%的AAP（初始浓度为1000 μg l⁻¹），且大部分AAP的还原发生在前5分钟。处理性能取决于高铁酸盐（VI）的剂量、pH值以及共存离子和腐殖酸的类型与强度。在最佳pH值7时增加高铁酸盐（VI）的剂量可提高AAP的降解率。在腐殖酸存在的情况下，高铁酸盐（VI）对AAP的降解在短时间内（<30分钟）得到促进，但随后随着腐殖酸含量的增加而受到抑制。Al³⁺、CO₃²⁻和PO₄³⁻离子的存在会降低AAP的去除率，但K⁺、Na⁺、Mg²⁺和Ca²⁺离子的存在可提高AAP的去除效果。发现了Al³⁺对水溶液中高铁酸盐（VI）分解的催化作用。高铁酸盐（VI）与AAP反应的动力学对高铁酸盐（VI）为假一级反应，对AAP为假二级反应。高铁酸盐（VI）与AAP的假速率常数为1.4×10⁻⁵ L² mg⁻² min⁻¹。鉴定出了三种氧化产物（OPs）并提出了AAP的降解途径。
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