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多溴二苯醚的镍/铁双金属纳米颗粒脱溴:影响因素、动力学和机制。

Debromination of polybrominated diphenyl ethers by Ni/Fe bimetallic nanoparticles: influencing factors, kinetics, and mechanism.

机构信息

School of Chemistry and Environment, South China Normal University, Guangzhou 510006, China.

出版信息

J Hazard Mater. 2011 Jan 30;185(2-3):958-69. doi: 10.1016/j.jhazmat.2010.09.113. Epub 2010 Oct 8.

Abstract

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.

摘要

多溴联苯醚已被确定为一类具有生态风险的新型有机污染物,因为它们具有毒性、生物蓄积性和全球分布性。需要适当的修复技术来从环境中去除它们。在本文中,通过化学沉积合成了 Ni/Fe 双金属纳米粒子,并将其用于降解十溴联苯醚 (BDE209)。通过透射电子显微镜、X 射线衍射、X 射线光电子能谱和 Brunnaer-Emmett-Teller 表面积分析对 Ni/Fe 纳米粒子的特性进行了分析。直径在 20-50nm 左右的 Ni/Fe 双金属纳米粒子可以有效地在溶剂(四氢呋喃/水)中降解 BDE209。研究了 Ni/Fe 纳米粒子用量、初始 BDE209 浓度和 Ni 负载等因素对 BDE209 去除的影响。结果表明,BDE209 的降解遵循拟一级动力学,BDE209 的降解速率随着纳米 Ni/Fe 颗粒、Ni/Fe 比的增加和初始 BDE209 浓度的降低而增加。通过分析 BDE209 去除的质量平衡,降解是 BDE209 去除的主要过程。通过使用气相色谱-质谱分析反应产物,推断了脱溴的机理,溶液中的溴化物离子和改变溶剂条件。逐步氢还原是脱溴的主要过程,氢在反应中起着重要作用。此外,还进行了 Ni 的长期性能和浸出实验,以测试 Ni/Fe 纳米粒子在 BDE209 降解中的稳定性和耐久性。

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