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美国密歇根州马卡塔瓦湖沉积物中一种高抗性芳香胺的缓慢解吸行为。

Slow desorption behavior of one highly resistant aromatic amine in Lake Macatawa, Michigan, USA, sediment.

作者信息

Chen Shihua, Nyman Marianne C

机构信息

Department of Civil and Environmental Engineering, Rensselaer Polytechnic Institute, Troy, New York 12180, USA.

出版信息

Environ Toxicol Chem. 2005 Dec;24(12):3020-9. doi: 10.1897/05-017r.1.

Abstract

The desorption behavior of benzidine from Lake Macatawa (Holland, MI, USA) sediment was investigated in this study using batch solvent extraction method. Seven solvents were tested as the extracting reagents: Deionized water (DI), calcium chloride in DI (CaCl2), sodium hydroxide in DI (NaOH), acetonitrile (ACN), a mixture of acetonitrile and ammonium acetate in DI (ACN-NH4OAc), methanol (MeOH), and hydrochloric acid in DI (HCl). These solvents are proposed to react with sediment-associated benzidine by different mechanisms (e.g., cation exchange, hydrophobic partitioning, and covalent binding). Three sets of sorption isotherm experiments were conducted separately in these seven solvents with a 7-d, three-week, and two-month contact time. The results demonstrated nonlinear isotherms with Freundlich 1/n values varying from 0.25 to 0.52. The desorption behavior of benzidine in the solvents was evaluated after the sorption of benzidine onto the sediment with same contact times of 7 d, three weeks, and two months. A two-stage model subsequently was applied to simulate the experimental data. The rapidly desorbing rate constants were on the order of one to two per day for ACN, ACN-NH4OAc, and NaOH solvents, and the slowly desorbing rate constants were on the order of 10(-5) to 10(-4)/d. Sequential desorption experiment demonstrated low total extraction efficiency of less than 40%. Both the observed sorption and desorption phenomena suggested that hysteresis and/or mass-transfer limited diffusion may result in the slow desorption behavior observed in this study.

摘要

本研究采用批量溶剂萃取法,对来自美国密歇根州荷兰市马卡塔瓦湖沉积物中联苯胺的解吸行为进行了研究。测试了七种溶剂作为萃取剂:去离子水(DI)、DI中的氯化钙(CaCl2)、DI中的氢氧化钠(NaOH)、乙腈(ACN)、DI中乙腈和醋酸铵的混合物(ACN-NH4OAc)、甲醇(MeOH)以及DI中的盐酸(HCl)。这些溶剂被认为通过不同机制(如阳离子交换、疏水分配和共价结合)与沉积物结合的联苯胺发生反应。在这七种溶剂中分别进行了三组吸附等温线实验,接触时间分别为7天、三周和两个月。结果表明等温线呈非线性,弗伦德利希1/n值在0.25至0.52之间变化。在相同的7天、三周和两个月接触时间下,将联苯胺吸附到沉积物上后,评估了联苯胺在这些溶剂中的解吸行为。随后应用两阶段模型对实验数据进行模拟。对于ACN、ACN-NH4OAc和NaOH溶剂,快速解吸速率常数约为每天一到两个,缓慢解吸速率常数约为10^(-5)至10^(-4)/天。连续解吸实验表明总萃取效率较低,不到40%。观察到的吸附和解吸现象均表明,滞后和/或传质限制扩散可能导致本研究中观察到的缓慢解吸行为。

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