Journal
ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 50, Issue 14, Pages 7470-7479Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.6b02119
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Funding
- National 973 program [2015CB453100]
- National Natural Science Foundation of China [21477147]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB14020102]
- Youth Innovation Promotion Association Chinese Academy of Sciences [2016038]
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Heterogeneous reactions mediated by fly ash are important to polychlorinated dibenzo-p-dioxin and dibenzofuran (PCDD/Fs) formation. However, the formation of polybrominated dibenzo-p-dioxins and dibenzofurans (PBDD/Fs) through heterogeneous reactions is not yet well understood. Experiments were performed to investigate the thermochemical formation of PBDD/Fs at 150-450 degrees C through heterogeneous reactions on fly ash from a secondary copper smelter. The maximum PBDD/F concentration was 325 times higher than the initial PBDD/F concentration in the fly ash. The PBDD/F concentration after the experiment at 150 degrees C was five times higher than the initial concentration. PBDD/Fs have not previously been found to form at such a low temperature. Secondary-copper-smelter fly ash clearly promoted PBDD/F formation, and this conclusion was supported by the low activation energies that were found in Arrhenius's law calculations. Thermochemical formation of PBDD/Fs mediated by fly ash deposited in industrial facilities could explain memory effects that have been found for PCDD/Fs and similar compounds released from industrial facilities. Abundant polybrominated diphenyl ethers (PBDEs) that were formed through fly ash-mediated reactions could be important precursors for PBDD/Fs also formed through fly ash-mediated reactions. The amounts of PBDEs that formed through fly ash-mediated reactions suggested that secondary copper smelters could be important sources of reformed PBDEs.
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