Kinetics and pathways for the debromination of polybrominated diphenyl ethers by bimetallic and nanoscale zerovalent iron: effects of particle properties and catalyst.
Kinetics and pathways for the debromination of polybrominated diphenyl ethers by bimetallic and nanoscale zerovalent iron: effects of particle properties and catalyst.
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DOI：
10.1016/j.chemosphere.2012.05.078
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发表时间：
2012-10
期刊：
影响因子：
8.8
通讯作者：
Luthy RG
中科院分区：
文献类型：
--
作者：
Zhuang Y;Jin L;Luthy RG
多溴二苯醚 (PBDE) 被认为是一类新的广泛分布且持久的污染物，需要有效的处理和修复技术。在本研究中，使用两种市售纳米级 Fe° 浆料（Nanofer N25 和 N25S）、冷冻干燥的实验室合成 Fe° 纳米颗粒 (nZVI) 及其钯化形式来研究颗粒特性和催化剂对 PBDE 脱溴动力学和途径的影响。人们发现 Nanofers 及其钯化形式可以有效地脱溴 PBDE。实验室合成的 Fe° 纳米颗粒也能脱溴 PBDE，但由于实验室合成中的冷冻干燥和稳定过程导致失活，速度较慢。与 N25 相比，结合在 N25S 上的有机改性剂聚丙烯酸 (PAA) 可将 PBDE 脱溴减慢三到四倍。在我们的系统中，钯化 nZVI (nZVI/Pd) 的活性优化为 0.3 Pd/Fe wt%。 N25可以在一周内将环境丰富的PBDEs（包括BDE 209、183、153、99和47）脱溴为最终产品二BDE、单BDE和二苯醚（DE），而nZVI/Pd（0.3 Pd/Fe wt%）主要产生DE作为最终产品。描述并比较了未经修饰和钯化 Fe° 的逐步主要 PBDE 脱溴途径。表面前体络合物的形成是钯化 Fe° 还原的重要限制因素，PBDE 途径证明了这一点，其中空间位阻和相邻溴的快速连续脱溴发挥着重要作用。
Polybrominated diphenyl ethers (PBDEs) are recognized as a new class of widely-distributed and persistent contaminants for which effective treatment and remediation technologies are needed. In this study, two kinds of commercially available nanoscale Fe° slurries (Nanofer N25 and N25S), a freeze-dried laboratory-synthesized Fe° nanoparticle (nZVI), and their palladized forms were used to investigate the effect of particle properties and catalyst on PBDE debromination kinetics and pathways. Nanofers and their palladized forms were found to debrominate PBDEs effectively. The laboratory-synthesized Fe° nanoparticles also debrominated PBDEs, but were slower due to deactivation by the freeze-drying and stabilization processes in the laboratory synthesis. An organic modifier, polyacrylic acid (PAA), bound on N25S slowed PBDE debromination by a factor of three to four compared to N25. The activity of palladized nZVI (nZVI/Pd) was optimized at 0.3 Pd/Fe wt% in our system. N25 could debrominate selected environmentally-abundant PBDEs, including BDE 209, 183, 153, 99, and 47, to end products di-BDEs, mono-BDEs and diphenyl ether (DE) in one week, while nZVI/Pd (0.3 Pd/Fe wt%) mainly resulted in DE as a final product. Step-wise major PBDE debromination pathways by unamended and palladized Fe° are described and compared. Surface precursor complex formation is an important limiting factor for palladized Fe° reduction as demonstrated by PBDE pathways where steric hindrance and rapid sequential debromination of adjacent bromines play an important role.
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