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多溴二苯醚(PBDEs)的钯化零价锌颗粒脱溴:影响因素、途径和机制。

Debromination of polybrominated diphenyl ethers (PBDEs) by palladized zerovalent zinc particles: Influence factors, pathways and mechanism.

机构信息

School of Environment and Energy, South China University of Technology, Guangzhou, 510006, China.

School of Environment and Energy, South China University of Technology, Guangzhou, 510006, China; The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters, Ministry of Education, Guangzhou, 510006, China.

出版信息

Chemosphere. 2020 Aug;253:126726. doi: 10.1016/j.chemosphere.2020.126726. Epub 2020 Apr 9.

Abstract

We synthesized a novel material, namely palladized zero-valent zinc (Pd/ZVZ), and investigated its efficiency for the degradation of polybrominated diphenyl ethers (PBDEs). The plated Pd significantly enhances the degradation rate of PBDEs by ZVZ at the optimum loading of 1% by weight. In the Pd/ZVZ system, very few lower BDEs were accumulated during the degradation of 2,2',4,4'- tetrabromodiphenyl ether (BDE-47) and the final product is diphenyl ether, whereas the ZVZ system only debrominates BDE-47 to di-BDE and further debromination becomes very difficult. The degradation rates of BDEs by ZVZ greatly decreased with decreased bromination level, while in Pd/ZVZ system, the degradation rates of PBDEs did not show a significant difference. These indicate different mechanisms. This was confirmed by investigating the debromination pathways of the PBDEs in both systems. We determined that a H-transfer was the dominant mechanism in the Pd/ZVZ system. In addition, the reactivity of Pd/ZVZ to BDE-47 is pH-independent, which has a great advantage for various applications over ZVZ alone. Our study provides a new approach for the remediation of the PBDEs pollution.

摘要

我们合成了一种新型材料,即钯负载零价锌(Pd/ZVZ),并研究了其对多溴二苯醚(PBDEs)降解的效率。在最佳负载量为 1%(重量比)时,负载的 Pd 显著提高了 ZVZ 对 PBDEs 的降解速率。在 Pd/ZVZ 体系中,在 2,2',4,4'-四溴二苯醚(BDE-47)的降解过程中,很少有较低 BDEs 积累,最终产物是二苯醚,而 ZVZ 体系仅将 BDE-47 脱溴化为二溴二苯醚,进一步脱溴变得非常困难。ZVZ 体系中 BDEs 的降解速率随溴化程度的降低而大大降低,而在 Pd/ZVZ 体系中,PBDEs 的降解速率没有明显差异。这表明存在不同的机制。通过研究两种体系中 PBDEs 的脱溴途径,我们证实了这一点。我们确定 H 转移是 Pd/ZVZ 体系中的主要机制。此外,Pd/ZVZ 对 BDE-47 的反应性与 pH 无关,这使其在各种应用中相对于单独的 ZVZ 具有很大的优势。我们的研究为 PBDEs 污染的修复提供了一种新方法。

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