Low-temperature persulfate activation by powdered activated carbon for simultaneous destruction of perfluorinated carboxylic acids and 1,4-dioxane

被引:46
作者
Manz, Katherine E. [1 ]
Kulaots, Indrek [1 ]
Greenley, Caroline A. [1 ]
Landry, Patrick J. [2 ]
Lakshmi, K. V. [2 ]
Woodcock, Matthew J. [1 ]
Hellerich, Lucas [3 ]
Bryant, J. Daniel [4 ]
Apfelbaum, Mike [5 ]
Pennell, Kurt D. [1 ]
机构
[1] Brown Univ, Sch Engn, Providence, RI 02912 USA
[2] Rensselaer Polytech Inst, Baruch Ctr Biochem Solar Energy Res 60, Troy, NY 12180 USA
[3] Woodard & Curran, 213 Court St,4th Floor, Middletown, CT 06457 USA
[4] Woodard & Curran, 50 Millstone Rd,Bldg 400, East Windsor, NJ 08520 USA
[5] Woodard & Curran, 40 Shattuck Rd,Suite 110, Andover, MA 01810 USA
关键词
Persulfate; Powdered activated carbon (PAC); Perfluorooctanoic acid (PFOA); 4-dioxane; Spin trapping; DMPO radical adducts; In-situ chemical oxidation (ISCO); POLYFLUOROALKYL SUBSTANCES PFAS; IN-SITU TREATMENT; PERFLUOROOCTANOIC ACID; DEGRADATION; OXIDATION; HEAT; WATER; MECHANISM; ION; PEROXYMONOSULFATE;
D O I
10.1016/j.jhazmat.2022.129966
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Carbonaceous materials have emerged as a method of persulfate activation for remediation. In this study, per -sulfate activation using powdered activated carbon (PAC) was demonstrated at temperatures relevant to groundwater (5-25 degrees C). At room temperature, increasing doses of PAC (1-20 g L-1) led to increased persulfate activation (3.06 x 10-6s-1 to 2.10 x 10-4 with 1 and 20 g L-1 PAC). Activation slowed at lower temperatures (5 and 11 degrees C); however, substantial (>70 %) persulfate activation was achieved. PAC characterization showed that persulfate is activated at the surface of the PAC, as indicated by an increase in the PAC C:O ratio. Similarly, electron paramagnetic resonance (EPR) spectroscopy studies with a spin trapping agents (5,5-dimethyl-1-pyr-roline N-oxide (DMPO)) and 2,2,6,6-tetramethylpiperidine (TEMP) revealed that singlet oxygen was not the main oxidizing species in the reaction. DMPO was oxidized to form 5,5-dimethylpyrrolidone-2(2)-oxyl-(1) (DMPOX), which forms in the presence of strong oxidizers, such as sulfate radicals. The persulfate/PAC sys-tem is demonstrated to simultaneously degrade both perfluorooctanoic acid (PFOA) and 1,4-dioxane at room temperature and 11 degrees C. With a 20 g L-1 PAC and 75 mM persulfate, 80 % and 70 % of the PFOA and 1,4-dioxane, respectively, degraded within 6 h at room temperature. At 11 degrees C, the same PAC and persulfate doses led to 57% dioxane degradation and 54 % PFOA degradation within 6 h. Coupling PAC with persulfate offers an effective, low-cost treatment for simultaneous destruction of 1,4-dioxane and PFOA.
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页数:10
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