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超声辐照下制备的镍铁纳米颗粒对2,4-二氯苯酚的催化脱氯作用

Catalytic dechlorination of 2,4-dichlorophenol by Ni/Fe nanoparticles prepared in the presence of ultrasonic irradiation.

作者信息

Zhao Deming, Zheng Yiya, Li Min, Baig Shams Ali, Wu Donglei, Xu Xinhua

机构信息

College of Chemical Engineering and Materials Science, Zhejiang University of Technology, Hangzhou 310032, People's Republic of China.

College of Chemical Engineering and Materials Science, Zhejiang University of Technology, Hangzhou 310032, People's Republic of China; Ningbo Research and Design Institute of Chemical Industry, Ningbo 315040, People's Republic of China.

出版信息

Ultrason Sonochem. 2014 Sep;21(5):1714-21. doi: 10.1016/j.ultsonch.2014.03.002. Epub 2014 Mar 13.

Abstract

In this study, nickle/iron (Ni/Fe) nanoparticles were synthesized by liquid phase reductive method in the presence of 20 kHz ultrasonic irradiation to improve nanoparticles' disparity and avoid agglomeration. The characterized results showed that this method has obviously modified most of the particles in term of sizes and specific surface areas. Meanwhile, the improved nanoscale Ni/Fe particles were employed for the reductive dechlorination of 2,4-dichlorophenol (2,4-DCP) as a function of some influential factors (Ni content, Ni/Fe nanoparticles dosage, reaction temperature and initial pH values) and degradation path. Experimental results showed that 2,4-DCP was first adsorbed by Ni/Fe nanoparticles, then quickly reduced to o-chlorophenol (o-CP), p-chlorophenol (p-CP), and finally to phenol (P). The application of ultrasonic irradiation for Ni/Fe nanoparticles synthesis was found to significantly enhance the removal efficiency of 2,4-DCP. Consequently, the phenol production rates increased from 68% (in the absence of ultrasonic irradiation) to 87% (in the presence of ultrasonic irradiation) within 180 min. Nearly 96% of 2,4-DCP was removed after 300 min reaction with these optimized conditions: Ni content over Fe(0) 3 wt%, initial 2,4-DCP concentration 20 mg L(-1), Ni/Fe dosage 3 g L(-1), initial pH value 3.0, and reaction temperature 25 °C. The degradation of 2,4-DCP followed pseudo-first-order kinetics reaction and the apparent pseudo-first-order kinetics constant was 0.0737 min(-1). This study suggested that the presence of ultrasonic irradiation in the synthesis of nanoscale Ni/Fe particles could be a promising technique to enhance nanoparticle's disparity and avoid agglomeration.

摘要

在本研究中,通过液相还原法在20 kHz超声辐照下合成镍/铁(Ni/Fe)纳米颗粒,以改善纳米颗粒的分散性并避免团聚。表征结果表明,该方法在尺寸和比表面积方面对大多数颗粒有明显改性。同时,将改进后的纳米级Ni/Fe颗粒用于2,4-二氯苯酚(2,4-DCP)的还原脱氯,研究了一些影响因素(Ni含量、Ni/Fe纳米颗粒用量、反应温度和初始pH值)及其降解路径。实验结果表明,2,4-DCP首先被Ni/Fe纳米颗粒吸附,然后迅速还原为邻氯苯酚(o-CP)、对氯苯酚(p-CP),最终还原为苯酚(P)。研究发现,超声辐照用于合成Ni/Fe纳米颗粒可显著提高2,4-DCP的去除效率。因此,在180分钟内,苯酚生成率从68%(无超声辐照)提高到87%(有超声辐照)。在以下优化条件下反应300分钟后,近96%的2,4-DCP被去除:Ni含量超过Fe(0) 3 wt%,初始2,4-DCP浓度20 mg L(-1),Ni/Fe用量3 g L(-1),初始pH值3.0,反应温度25 °C。2,4-DCP的降解遵循准一级动力学反应,表观准一级动力学常数为0.0737 min(-1)。本研究表明,在纳米级Ni/Fe颗粒合成过程中引入超声辐照可能是一种提高纳米颗粒分散性并避免团聚的有前景的技术。

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