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4-苯乙酰苯腙功能化硅胶:一种新型螯合基质的合成及其作为金属离子捕集剂的应用

Silica gel functionalized with 4-phenylacetophynone 4-aminobenzoylhydrazone: Synthesis of a new chelating matrix and its application as metal ion collector.

作者信息

Hatay I, Gup R, Ersöz M

机构信息

Selcuk University, Chemistry Department, 42070 Campus, Konya, Turkey.

出版信息

J Hazard Mater. 2008 Feb 11;150(3):546-53. doi: 10.1016/j.jhazmat.2007.05.002. Epub 2007 May 6.

DOI:10.1016/j.jhazmat.2007.05.002
PMID:17566643
Abstract

The silica gel surface immobilized with 4-phenylacetophynone 4-aminobenzoylhydrazone (PAAH) after surface modification by 3-chloropropyltrimethoxysilane (CPTS). The modified silica gel was used for sorption of Cu(II), Ni(II) and Co(II) in aqueous solution. The effect of solution pH, sorption time, temperature and initial metal ion concentration onto metal ions sorption was investigated. The characteristics of the sorption process were evaluated by using the Langmuir, Freundlich and Dubinin-Radushkevich (D-R) adsorption isotherms. The sorption of metal ions onto modified silica gel correlated well with the Langmuir type adsorption isotherm and adsorption capacities were found to be 0.012, 0.014 and 0.018 mmol g(-1) for Cu(II), Ni(II) and Co(II) metal ions, respectively. From the D-R adsorption isotherms, it was concluded that chemical interactions and chelating effects were playing an important role in the sorption of metal ions onto modified silica gel. Thermodynamic parameters such as the standard free energy change (DeltaG) degrees , enthalpy change (DeltaH degrees ) and entrophy change (DeltaS degrees ) were calculated to determine the nature of sorption process. From these parameters, DeltaH degrees were found to be endothermic values: 38.39, 18.0, and 14.7 kJ mol(-1) for the same sequence of divalent cations and DeltaS degrees values were calculated to be positive for the sorption of each metal ion onto the modified silica gel. Negative DeltaG degrees values indicated that sorption process for all metal ions were spontaneous in nature although they presented an endothermic enthalpy for the interaction, resulting in an entropically favoured process.

摘要

硅胶表面经3-氯丙基三甲氧基硅烷(CPTS)进行表面改性后,固定有4-苯基乙酰苯腙(PAAH)。改性硅胶用于吸附水溶液中的Cu(II)、Ni(II)和Co(II)。研究了溶液pH值、吸附时间、温度和初始金属离子浓度对金属离子吸附的影响。通过Langmuir、Freundlich和Dubinin-Radushkevich(D-R)吸附等温线对吸附过程的特征进行了评估。金属离子在改性硅胶上的吸附与Langmuir型吸附等温线相关性良好,发现Cu(II)、Ni(II)和Co(II)金属离子的吸附容量分别为0.012、0.014和0.018 mmol g(-1)。从D-R吸附等温线得出结论,化学相互作用和螯合效应在金属离子在改性硅胶上的吸附中起重要作用。计算了标准自由能变化(ΔG°)、焓变(ΔH°)和熵变(ΔS°)等热力学参数,以确定吸附过程的性质。从这些参数中发现,对于相同顺序的二价阳离子,ΔH°为吸热值:分别为38.39、18.0和14.7 kJ mol(-1),并且计算得出每个金属离子在改性硅胶上的吸附的ΔS°值为正值。负的ΔG°值表明,尽管所有金属离子的吸附过程在相互作用时呈现吸热焓,但本质上都是自发的,导致了一个熵有利的过程。

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