TY - JOUR
T1 - IMPACT
T2 - Innovative (nano)Materials and processes for advanced catalytic technologies to degrade PFOA in water
AU - Osonga, Francis J.
AU - Eshun, Gaddi B.
AU - Xue, Huize
AU - Kurilla, Stephen
AU - Al Hassan, Md Tanim
AU - Qamar, Areej
AU - Chen, Hao
AU - Boufadel, Michel
AU - Sadik, Omowunmi A.
N1 - Publisher Copyright:
© 2024 Elsevier Ltd
PY - 2024/9
Y1 - 2024/9
N2 - We hereby report the development of a novel electrochemical method to degrade perfluorooctanoic acid (C7F15COOH, PFOA). At the center of the approach are bimetallic Pd–Ru nano-catalyst materials called IMPACT: Innovative (nano)Materials and Processes for Advanced Catalytic Technologies. IMPACT uses flavonoid-sequestered Pd–Ru, allowing the development of specialized electrodes with tunable properties to sequentially degrade PFOA in wastewater samples into a sustainable byproduct via an indirect electrochemical method. Electron transfers at RuOxHy species stabilize the Pd component of the nano-catalysts, enabling the degradation process via PFOA deprotonation, chain shortening, decarboxylation, hydrolysis, fluoride elimination, and CF2 flake-off mechanism. IMPACT enabled the observation of redox peaks at −0.26 V and 0.56 V for the first time, with accompanying reduction peaks at −0.5V and 0.29 V, respectively. These redox peaks, which correlated with the concentrations of PFOA (20, 50, 100, 200, and 400. mg L−1), were verified and confirmed using electrochemical simulations. Control experiments did not show degradation of PFOA in the absence of Pd–Ru nano-catalyst. The degradation in wastewater was obtained within 3 h with an efficiency of 98.5%. The electrochemical degradation products of PFOA were identified using High-resolution desalting paper spray mass spectrometry (DPS-MS) and collision-induced dissociation (CID) analysis. The results yielded C2F5COOH, C3F7COOH, and C6F13OH with dissociation losses of CF2O or CO2. IMPACT introduces a novel nano-catalyst with high efficiency and a reliable capability that defluorinates strong C–F bonds that are components of recalcitrant organics in myriad environmental matrices.
AB - We hereby report the development of a novel electrochemical method to degrade perfluorooctanoic acid (C7F15COOH, PFOA). At the center of the approach are bimetallic Pd–Ru nano-catalyst materials called IMPACT: Innovative (nano)Materials and Processes for Advanced Catalytic Technologies. IMPACT uses flavonoid-sequestered Pd–Ru, allowing the development of specialized electrodes with tunable properties to sequentially degrade PFOA in wastewater samples into a sustainable byproduct via an indirect electrochemical method. Electron transfers at RuOxHy species stabilize the Pd component of the nano-catalysts, enabling the degradation process via PFOA deprotonation, chain shortening, decarboxylation, hydrolysis, fluoride elimination, and CF2 flake-off mechanism. IMPACT enabled the observation of redox peaks at −0.26 V and 0.56 V for the first time, with accompanying reduction peaks at −0.5V and 0.29 V, respectively. These redox peaks, which correlated with the concentrations of PFOA (20, 50, 100, 200, and 400. mg L−1), were verified and confirmed using electrochemical simulations. Control experiments did not show degradation of PFOA in the absence of Pd–Ru nano-catalyst. The degradation in wastewater was obtained within 3 h with an efficiency of 98.5%. The electrochemical degradation products of PFOA were identified using High-resolution desalting paper spray mass spectrometry (DPS-MS) and collision-induced dissociation (CID) analysis. The results yielded C2F5COOH, C3F7COOH, and C6F13OH with dissociation losses of CF2O or CO2. IMPACT introduces a novel nano-catalyst with high efficiency and a reliable capability that defluorinates strong C–F bonds that are components of recalcitrant organics in myriad environmental matrices.
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U2 - 10.1016/j.chemosphere.2024.143057
DO - 10.1016/j.chemosphere.2024.143057
M3 - Article
C2 - 39146983
AN - SCOPUS:85201469552
SN - 0045-6535
VL - 364
JO - Chemosphere
JF - Chemosphere
M1 - 143057
ER -