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Front. Environ. Sci. Eng.    2020, Vol. 14 Issue (3) : 47    https://doi.org/10.1007/s11783-020-1224-2
RESEARCH ARTICLE
Enhanced debromination of 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47) by zero-valent zinc with ascorbic acid
Chaojin Jiang1,2, Xiaoqian Jiang1,2, Lixun Zhang1,2, Yuntao Guan1,2()
1. Guangdong Provincial Engineering Technology Research Center for Urban Water Cycle and Water Environment Safety, Tsinghua Shenzhen International Graduate School, Shenzhen 518055, China
2. State Environmental Protection Key Laboratory of Microorganism Application and Risk Control, School of Environment, Tsinghua University, Beijing 100084, China
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Abstract

• Highly efficient debromination of BDE-47 was achieved in the ZVZ/AA system.

• BDE-47 debromination by the ZVZ/AA can be applied to a wide range of pH.

• AA inhibits the formation of (hydr)oxide and accelerates the corrosion of ZVZ.

• Reduction mechanism of BDE-47 debromination by the ZVZ/AA system was proposed.

A new technique of zero-valent zinc coupled with ascorbic acid (ZVZ/AA) was developed and applied to debrominate the 2,2′,4,4′-Tetrabromodiphenyl ether (BDE-47), which achieved high conversion and rapid debromination of BDE-47 to less- or non-toxic forms. The reaction conditions were optimized by the addition of 100 mg/L ZVZ particles and 3 mmol/L AA at original solution pH= 4.00 using the solvent of methanol/H2O (v:v= 4:6), which could convert approximately 94% of 5 mg/L BDE-47 into lower-brominated diphenyl ethers within a 90 min at the ZVZ/AA system. The high debromination of BDE-47 was mainly attributed to the effect of AA that inhibits the formation of Zn(II)(hydr)oxide passivation layers and promotes the corrosion of ZVZ, which leads to increase the reactivity of ZVZ. Additionally, ion chromatography and gas chromatography mass spectrometry analyses revealed that bromine ion and lower-debromination diphenyl ethers formed during the reduction of BDE-47. Furthermore, based on the generation of the intermediates products, and its concentration changes over time, it was proposed that the dominant pathway for conversion of BDE-47 was sequential debromination and the final products were diphenyl ethers. These results suggested that the ZVZ/AA system has the potential for highly efficient debromination of BDE-47 from wastewater.
Keywords 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47)      Ascorbic acid      Reductive debromination      Zero-valent zinc     
Corresponding Author(s): Yuntao Guan   
Just Accepted Date: 13 February 2020   Issue Date: 13 March 2020
 Cite this article:   
Chaojin Jiang,Xiaoqian Jiang,Lixun Zhang, et al. Enhanced debromination of 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47) by zero-valent zinc with ascorbic acid[J]. Front. Environ. Sci. Eng., 2020, 14(3): 47.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-020-1224-2
https://academic.hep.com.cn/fese/EN/Y2020/V14/I3/47
Fig.1  Effect of different systems on BDE-47 conversion (100 mg/L ZVZ, 3 mmol/L AA, methanol/H2O= 40/60 (v/v), and pH= 4.00).
BDE-47 initial concentration Metal reductant and dosage Operating conditions Conversion time and efficiency Conversion kinetics: kobs (h−1) Refs.
200 µg/L (methanol/water solvent) Fe/Pd 60±3 g/L
Fe 60±3 g/L		 60 r/min
60 r/min		 15 min, 31%
2 d, 2.7%		 0.48
0.09		 Zhuang et al.(2012)
2 mg/L (methanol/water solvent, 50/50) Attapulgite-supported Fe/Ni bimetallic nanoparticles, 3 g/L 250 r/min
pH 4.00		 480 min, 90% 0.44 Liu et al.(2015)
5 mg/L aqueous solution Fe/Ag nanoparticles, 1 g/L Ultrasound (40 kHz and 100 W) as 25°C±2°C 120 min, 99% 0.65 Luo et al.(2011)
5 mg/L (methanol/water solvent, 40/60) ZVZ/AA 100 mg/L+ 3 mmol/L
ZVZ 100 mg/L
AA 3 mmol/L		 pH 4.00
250 r/min		 90 min, 94%
90 min, 68%
90 min, 14%		 1.78
0.74
0.084		 This work
Tab.1  Conversion efficiency and observed pseudo first-order rate constants (kobs) of BDE-47 under various reduction conditions as described in previous reports
Fig.2  XRD patterns for ZVZ: (a) after reaction of ZVZ/AA system, (b) after reaction of ZVZ system, and (c) before reaction.
Fig.3  SEM image of ZVZ: (a) before reaction, (b) after reaction of ZVZ system, (c) and (d) after reaction of ZVZ/AA system.
Fig.4  The proposed mechanisms in the ZVZ/AA system for the conversion of BDE-47.
Fig.5  Effect of water proportion on BDE-47 conversion (100 mg/L ZVZ, 3 mmol/L AA, and pH= 4.00)
Fig.6  Effect of (a) ZVZ dosage (fixed AA: 3 mmol/L) and (b) AA addition amount (fixed ZVZ dosage: 100 mg/L) on BDE-47 conversion in acidic solution (methanol/H2O= 40/60 (v/v), pH= 4.00).
Fig.7  Effect of original solution pH on BDE-47 conversion (100 mg/L ZVZ, 3 mmol/L AA and methanol/H2O= 40/60 (v/v)).
Fig.8  (a) Debromination rate of BDE-47 by ZVZ, AA, and ZVZ/AA system (100 mg/L ZVZ, 3 mmol/L AA, methanol/H2O= 40/60 (v/v), and pH= 4.00); (b) Typical reaction profile and mass C-balance during the conversion process of BDE-47 with ZVZ/AA (100 mg/L ZVZ, 3 mmol/L AA, methanol/H2O= 40/60 (v/v), and pH= 4.00); (c) The proposed stepwise debromination pathway of BDE-47 in the ZVZ/AA system.
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