Debromination of polybrominated diphenyl ethers by Ni/Fe bimetallic nanoparticles: Influencing factors, kinetics, and mechanism
Debromination of polybrominated diphenyl ethers by Ni/Fe bimetallic nanoparticles: Influencing factors, kinetics, and mechanism
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DOI：
10.1016/j.jhazmat.2010.09.113
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发表时间：
2011-01-30
影响因子：
13.6
通讯作者：
Qiu, Xiuqi
中科院分区：
文献类型：
--
作者：
Fang, Zhanqiang;Qiu, Xinhong;Qiu, Xiuqi
多溴联苯醚因其毒性、生物蓄积性和全球性分布而被确定为一类新的具有生态风险的有机污染物。需要适当的补救技术才能将它们从环境中移除。在这篇论文中。采用化学沉积法制备了Ni/Fe双金属纳米粒子，并将其用于降解十溴二苯醚(BDE209)。通过透射电子显微镜、X射线衍射仪、X射线光电子能谱和Brunner-Emmett-Teller比表面积分析等手段对Ni/Fe纳米粒子的性能进行了分析。在四氢呋喃/水体系中，直径为20~50 nm的Ni/Fe双金属纳米粒子能有效地降解BDE209。考察了Ni/Fe纳米粒子投加量、BDE209初始浓度、镍负载量等因素对BDE209去除效果的影响。结果表明，BDE209的降解遵循准一级动力学，降解速率随纳米Ni/Fe粒子的加入量、Ni/Fe比的增加和BDE209初始浓度的降低而增加。通过对BDE209去除过程的质量平衡分析，认为降解是BDE209去除的主要过程。通过对反应产物、溶液中的溴离子以及改变溶剂条件的分析，推测了脱溴反应的机理。分步氢气还原是脱溴反应的主要过程，氢离子在反应中起着重要的作用。此外，还进行了镍的长期性能实验和镍的浸出实验，以测试镍/铁纳米粒子在BDE209降解中的稳定性和持久性。(C)2010爱思唯尔B.V.保留所有权利。
Polybrominated diphenyl ethers have been identified as a new class of organic pollutants with ecological risk due to their toxicity, bioaccumulation, and global distribution. Proper remediation technologies are needed to remove them from the environment. In this paper. Ni/Fe bimetallic nanoparticles were synthesized by chemical deposition and used to degrade decabromodiphenyl ether (BDE209). The characteristics of Ni/Fe nanoparticles were analyzed by transmission electron microscopy, X-ray diffractometry, X-ray photoelectron spectroscopy, and Brunnaer-Emmett-Teller surface area analysis. Ni/Fe bimetallic nanoparticles with diameters in the order of 20-50 nm could effectively degrade BDE209 in the solvent (tetrahydrofuran/water). Influence factors, such as Ni/Fe nanoparticle dosage, initial BDE209 concentration, and Ni loading, on the removal of BDE209 were studied. The results indicated that the degradation of BDE209 followed pseudo-first-order kinetics, and the degradation rate of BDE209 increased with increasing the amount of nano Ni/Fe particles, Ni/Fe ratio, and decreasing the initial concentration of BDE209. Through analyzed the mass balance of the BDE209 removal, degradation was the main process of BDE209 removal. The mechanism of debromination was deduced by analyzing the reaction products using gas chromatography-mass spectrometry, the bromide ion in the solution and varying the solvent conditions. Stepwise hydrogen reduction is the main process of debromination, and the hydrion play an important role in the reaction. Moreover, the experiment of long term performance and leaching of Ni were also carried out to test the stability and durability of Ni/Fe nanoparticles in BDE209 degradation. (C) 2010 Elsevier B.V. All rights reserved.