TY - JOUR
T1 - Decomposition of perfluorooctanic acid by carbon aerogel with persulfate
AU - Lee, Yu Chi
AU - Li, Yueh Feng
AU - Lo, Shang Lien
AU - Kuo, Jeff
AU - Sun, Wenjie
AU - Hu, Ching Yao
N1 - Funding Information:
This work was financially supported by National Taiwan University from Excellence Research Program-Core Consortiums (NTUCCP-107L891301, NTU-108L8806), and NTU Research Center for Future Earth from The Featured Areas Research Center Program within the framework of the Higher Education Sprout Project by the Ministry of Education (MOE) in Taiwan, and the Ministry of Science and Technology of the Republic of China (MOST 108-2621-M-002-024-MY2).
Publisher Copyright:
© 2021 Elsevier B.V.
PY - 2022/2/15
Y1 - 2022/2/15
N2 - Thermally-activated persulfate (PS) has been recognized as one of the most effective Advanced oxidation processes (AOPs) to oxidize Persistent perfluorooctanoic acid (PFOA). Applications of Carbon aerogel (CA)-activated PS for PFOA decomposition at 25, 40, 50 and 60 °C were evaluated. With the presence of CA in PS oxidation, 85.7% of PFOA was decomposed to fluoride ions and intermediates of short-chain perfluorinated carboxylic acids (PFCAs) with a 34.5% defluorination efficiency at 60 °C after 8 h. PFOA was decomposed and mineralized to fluoride ions in the CA + PS system following a stepwise degradation process of C6F13COOH → C5F11COOH → C4F9COOH → C3F7COOH → C2F5COOH → CF3COOH at 60 °C. The decomposition and defluorination rates of the combined CA + PS system at 60 °C were approximately 1.83 and 1.61 times faster than those of the PS-only system, respectively. With CA in the PS system, activation energies of PFOA removal and defluorination were significantly reduced from 66.8 to 37.2 and 97.3 to 49.2 kJ/mol, respectively. It implies that applying CA could effectively promote the PFOA degradation that leads to significant savings in energy consumption and reductions in process time. Characteristics of CA used were evaluated by using N2 adsorption, zeta potential, Raman, SEM, XRD, XPS and FT-IR techniques. A quenching test was conducted by using methanol as an inhibitor and Electron spin resonance (ESR) spectra of free radicals were analyzed for development of proposed reaction mechanisms.
AB - Thermally-activated persulfate (PS) has been recognized as one of the most effective Advanced oxidation processes (AOPs) to oxidize Persistent perfluorooctanoic acid (PFOA). Applications of Carbon aerogel (CA)-activated PS for PFOA decomposition at 25, 40, 50 and 60 °C were evaluated. With the presence of CA in PS oxidation, 85.7% of PFOA was decomposed to fluoride ions and intermediates of short-chain perfluorinated carboxylic acids (PFCAs) with a 34.5% defluorination efficiency at 60 °C after 8 h. PFOA was decomposed and mineralized to fluoride ions in the CA + PS system following a stepwise degradation process of C6F13COOH → C5F11COOH → C4F9COOH → C3F7COOH → C2F5COOH → CF3COOH at 60 °C. The decomposition and defluorination rates of the combined CA + PS system at 60 °C were approximately 1.83 and 1.61 times faster than those of the PS-only system, respectively. With CA in the PS system, activation energies of PFOA removal and defluorination were significantly reduced from 66.8 to 37.2 and 97.3 to 49.2 kJ/mol, respectively. It implies that applying CA could effectively promote the PFOA degradation that leads to significant savings in energy consumption and reductions in process time. Characteristics of CA used were evaluated by using N2 adsorption, zeta potential, Raman, SEM, XRD, XPS and FT-IR techniques. A quenching test was conducted by using methanol as an inhibitor and Electron spin resonance (ESR) spectra of free radicals were analyzed for development of proposed reaction mechanisms.
KW - Activation energy
KW - Carbon aerogel
KW - Defluorination
KW - Perfluorooctanoic acid
KW - Persulfate
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U2 - 10.1016/j.cej.2021.132900
DO - 10.1016/j.cej.2021.132900
M3 - Article
AN - SCOPUS:85117798029
SN - 1385-8947
VL - 430
JO - Chemical Engineering Journal
JF - Chemical Engineering Journal
M1 - 132900
ER -