TY - JOUR
T1 - Rapid transformation of 1,2,3,4-TCDD by Pd/Fe catalysts
AU - Wang, Zhiyuan
AU - Huang, Weilin
AU - Peng, Ping'an
AU - Fennell, Donna E.
N1 - Funding Information:
The authors sincerely thank Dr. Fang Liu and Professor Max M. Häggblom of Rutgers University for their assistance during the experimental phase of this study. We also thank Professor Häggblom for sharing analytical equipment and laboratory facilities. A graduate fellowship was provided by the Chinese Academy of Sciences to the first author (ZW) for this study at Rutgers University. The financial support was provided in part by the US National Science Foundation with an SGER Grant ( BES-0636820 ) to WH and the Strategic Environmental Research and Development Program of the Department of Defense with a grant to DEF.
PY - 2010/1
Y1 - 2010/1
N2 - This study investigated reductive dechlorination of 1,2,3,4-tetrachlorodibenzo-p-dioxin (1,2,3,4-TCDD) in the presence of Pd/Fe, Cu/Fe and Ni/Fe bimetallic catalysts or zero-valent iron (ZVI) under aqueous and ambient temperature conditions. It was found that the Pd/Fe catalyst can rapidly transform 1,2,3,4-TCDD to chlorine-free dibenzo-p-dioxin (DD) with >95% of conversion and half lives on the order of 5 h, whereas Cu/Fe, Ni/Fe and ZVI were not reactive over 10 d. The dechlorination of 1,2,3,4-TCDD in the Pd/Fe systems was found to be stepwise, with 1,2,3-tri (TrCDD), 1,2-di (DCDD), and mono-(MCDD) chlorodibenzo-p-dioxins as the three intermediate products at low concentrations and DD as the final and dominant product. The reaction rate of 1,2,3,4-TCDD dechlorination appeared to decrease as the coverage of palladium on iron particle surface increases from 0.0060 mol% to 0.0228 mol%. Compared to our prior study of reductive dechlorination of 1,2,3,4-TCDD with zero valent zinc (ZVZ) as the reductant, the reactions with Pd/Fe bimetallic materials were relatively slower for TCDD, but much faster for TrCDDs and DCDDs, yielding DD as the major product. The study suggested that Pd/Fe bimetallic catalyst-based reactions may be suitable for rapid decontamination of polychlorinated dibenzo-p-dioxin/dibenzofuran (PCDD/F) polluted soils and sediments.
AB - This study investigated reductive dechlorination of 1,2,3,4-tetrachlorodibenzo-p-dioxin (1,2,3,4-TCDD) in the presence of Pd/Fe, Cu/Fe and Ni/Fe bimetallic catalysts or zero-valent iron (ZVI) under aqueous and ambient temperature conditions. It was found that the Pd/Fe catalyst can rapidly transform 1,2,3,4-TCDD to chlorine-free dibenzo-p-dioxin (DD) with >95% of conversion and half lives on the order of 5 h, whereas Cu/Fe, Ni/Fe and ZVI were not reactive over 10 d. The dechlorination of 1,2,3,4-TCDD in the Pd/Fe systems was found to be stepwise, with 1,2,3-tri (TrCDD), 1,2-di (DCDD), and mono-(MCDD) chlorodibenzo-p-dioxins as the three intermediate products at low concentrations and DD as the final and dominant product. The reaction rate of 1,2,3,4-TCDD dechlorination appeared to decrease as the coverage of palladium on iron particle surface increases from 0.0060 mol% to 0.0228 mol%. Compared to our prior study of reductive dechlorination of 1,2,3,4-TCDD with zero valent zinc (ZVZ) as the reductant, the reactions with Pd/Fe bimetallic materials were relatively slower for TCDD, but much faster for TrCDDs and DCDDs, yielding DD as the major product. The study suggested that Pd/Fe bimetallic catalyst-based reactions may be suitable for rapid decontamination of polychlorinated dibenzo-p-dioxin/dibenzofuran (PCDD/F) polluted soils and sediments.
KW - PCDD
KW - Pd/Fe catalyst
KW - Reaction kinetics
KW - Reductive dechlorination
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UR - http://www.scopus.com/inward/citedby.url?scp=71949096811&partnerID=8YFLogxK
U2 - 10.1016/j.chemosphere.2009.09.066
DO - 10.1016/j.chemosphere.2009.09.066
M3 - Article
C2 - 19889441
AN - SCOPUS:71949096811
SN - 0045-6535
VL - 78
SP - 147
EP - 151
JO - Chemosphere
JF - Chemosphere
IS - 2
ER -