Journal
SCIENCE OF THE TOTAL ENVIRONMENT
Volume 661, Issue -, Pages 18-26Publisher
ELSEVIER SCIENCE BV
DOI: 10.1016/j.scitotenv.2019.01.166
Keywords
PBDEs; Zerovalent iron; Bimetallic particles; Electron transfer; H-atom transfer
Categories
Funding
- National Natural Science Foundation of China [41573091, 41771346, U1501234]
- Guangdong Natural Science Funds for Distinguished Young Scholar [2015A030306005]
- Tip-top Scientific and Technical Innovative Youth Talents of Guangdong Special Support Program [2015TQ01Z233]
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This study investigated the relative significance of electron transfer (e-transfer) and H-atom transfer (H-transfer) in a nanoscale zerovalent iron (n-ZVI) system and six n-ZVI-based bimetallic systems (Fe/Cu, Fe/Ni, Fe/Pd, Fe/Ag, Fe/Pt, and Fe/Au) through a case study of the debromination of 2,2', 4,4'-tetrabromodiphenyl ether (BDE-47). The results revealed that the reactivities of these bimetallic particles to BDE-47 decreased in the following order: Fe/Pd > Fe/Ag > Fe/Cu > Fe/Ni > Fe/Au > Fe/Pt approximate to n-ZVI. Debromination of BDE-47 in metal-H2 systems suggested that Ni, Pd, Pt, Cu and Au can utilize H-2 to debrominate BDE-47. In the H-transfer process, BDE-47 preferentially debrominated the para-bromine substituent to generate BDE-17, whereas in the e-transfer process, BDE-47 preferentially debrominate ortho-bromine substituent to generate BDE-28. The debromination pathways of BDE-47 in bimetallic and NaBH4-metal systems suggested that Fe/Ni, Fe/Pd and Fe/Pt debrominate polybrominated diphenyl ethers (PBDEs) through a H-transfer dominant mechanism, while Fe/Ag debrominate PBDEs through an e-transfer dominant mechanism. In the cases of Fe/Cu and Fe/Au, the e-transfer and H-transfer may be equally involved in the debromination of PBDEs. These results greatly improve our understanding of the relative significance of e-transfer and H-transfer in the dehalogenation of halogenated aromatic compounds (HACs) in various n-ZVI-based bimetallic systems. (C) 2019 Elsevier B.V. All rights reserved.
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