New insight into the cosolvent effect on the degradation of tetrabromobisphenol A (TBBPA) over millimeter-scale palladised sponge iron (Pd-s-Fe0) particles

作者：Huang, Zheng; Deng, Dongyang; Qiao, Junqin; Ju, Yongming^*; Chen, Yaling; Dionysiou, Dionysios D.^*

来源：Chemical Engineering Journal, 2019, 361: 1423-1436.

DOI：10.1016/j.cej.2018.10.203

• Debromination reactions
• Degradation mechanism
• nZVI
• Palladised (Pd) bimetals
• O-methylation reactions

The exploration of an effective treatment is necessary to eliminate the emerging environmental pollutant tetrabromobisphenol A (TBBPA). In this study, a direct reduction reaction was adopted to synthesize millimetre-scale palladised sponge iron (Pd-0-s-Fe-0), the main influencing factors were further explored, the degradation intermediates were identified in detail, and the cosolvent effect on the degradation mechanism was determined. The results show that (1) within a 30 min reaction, Pd(II) ions in aqueous solution were successfully decorated onto the s-Fe-0 surface as supported by XPS, SEM, EDS, and ICP-OES analyses, (2) after 120 min of reaction, the normalized removal of TBBPA was similar to 92.2% over 0.06 wt%-Pd-0-s-Fe-0, compared with 98.2% over 0.06 wt%-Pd-nZVI and 44.4% over bare nZVI. Moreover, the extend of debromination of TBBPA surprisingly increased as the ratio of the CH3OH: H2O cosolvent decreased, compared with the debromination rates that were greatly restricted in CH3OH (100%, v/v), CH2Cl2 (100%, v/v) and isopropanol (100%, v/v), respectively. Furthermore, the O-methylation reactions over Pd-0-s-Fe-0 produced unique intermediates, including 2,6-dibromo-4-(2-(3,5-dibromo-4-methoxyphenyl) propan-2-yl) phenol (MeO-TBBPA) and 5,5'-(propane-2,2-diyl) bis(1,3-dibromo-2-methoxy-benzene) (diMeO-TBBPA) with lower toxicity. This study greatly enriches knowledge regarding the degradation mechanism of TBBPA over millimetre-scale sponge iron.

• 出版日期2019-4-1
• 单位环境保护部华南环境科学研究所; 南京大学