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电化学顺序还原-氧化高效降解四溴双酚 A:降解效率、中间产物和途径。

Efficient degradation of tetrabromobisphenol A via electrochemical sequential reduction-oxidation: Degradation efficiency, intermediates, and pathway.

机构信息

School of Environment, Guangxi University, Nanning 530004, PR China.

School of Environment, Guangxi University, Nanning 530004, PR China.

出版信息

J Hazard Mater. 2018 Feb 5;343:376-385. doi: 10.1016/j.jhazmat.2017.10.004. Epub 2017 Oct 4.

DOI:10.1016/j.jhazmat.2017.10.004
PMID:29017121
Abstract

Tetrabromobisphenol A (TBBPA), a toxic persistent pollutant, should be effectively removed from the environment. In this study, an electrochemical sequential reduction-oxidation system was proposed by controlling reaction atmosphere with Pd-Fe nanoparticles modified Ni foam (Pd-Fe/Ni) electrode as cathode for TBBPA degradation. To obtain an efficient Pd-Fe/Ni electrode for TBBPA degradation, various factors, like Pd loading, Fe adding amounts, were examined. The Pd-Fe/Ni electrode exhibited higher TBBPA conversion and debromination than the counterparts, due to the synergism of Fe and electrochemical reduction. Similar TBBPA conversions and debromination ratios were observed for the cases of sparging N only and sparging N followed by air, which were higher than those of aeration. Reductive debromination occurred while first bubbling N, forming tri-BBPA, di-BBPA, mono-BBPA and BPA; and these intermediates were likely to be further oxidized by OH generated from HO together with Pd-Fe/Ni electrode under aeration. Reductive and oxidative intermediates (including aromatic ring-opened product) were identified by HPLC and UPLC-QTOF-MS. Based on the intermediates, the possible TBBPA degradation mechanism and pathway were proposed. This study demonstrates that sequential reduction-oxidation process tuned by N and air bubbling was favored for TBBPA degradation, thus, it should be a promising process for HOCs degradation.

摘要

四溴双酚 A(TBBPA)是一种有毒的持久性污染物,应从环境中有效去除。在这项研究中,通过控制反应气氛,采用 Pd-Fe 纳米颗粒修饰的 Ni 泡沫(Pd-Fe/Ni)电极作为阴极,提出了一种电化学顺序还原-氧化体系,用于 TBBPA 降解。为了获得用于 TBBPA 降解的高效 Pd-Fe/Ni 电极,研究了 Pd 负载量、Fe 添加量等各种因素。Pd-Fe/Ni 电极由于 Fe 的协同作用和电化学还原作用,表现出更高的 TBBPA 转化率和脱溴率。仅鼓泡 N 和先鼓泡 N 后鼓泡空气的情况下,TBBPA 的转化率和脱溴率与曝气的情况相似,均高于曝气的情况。首次鼓泡 N 时发生还原脱溴,形成三溴双酚 A、二溴双酚 A、单溴双酚 A 和 BPA;这些中间产物可能在曝气条件下与 Pd-Fe/Ni 电极一起由 HO 产生的 OH 进一步氧化。通过 HPLC 和 UPLC-QTOF-MS 鉴定了还原和氧化中间产物(包括芳环开环产物)。根据中间产物,提出了 TBBPA 降解的可能机制和途径。本研究表明,通过 N 和空气鼓泡调节的顺序还原-氧化过程有利于 TBBPA 降解,因此,它应该是一种有前途的 HOCs 降解过程。

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