Project 2: Integration of Remediation Technologies and Elucidation of Degradation Mechanisms

Prof. Yang Yang, PI
Prof. Yang Yang, PI
Prof. Jinyong Liu, PI
Prof. Jinyong Liu, PI

There is a pressing need for eradicating PFAS in contaminated water and soil for Superfund site remediation. The ideal treatment technology should be effective with most PFAS compounds and achieve complete defluorination (i.e., 100% of the C−F bonds cleaved into F− ions). However, current technologies for aqueous sample treatment have limitations in the (i) scope of treatable PFAS structures, (ii) extent of defluorination, and (iii) cost-effectiveness. Studies on the treatment of PFAS-laden solids, such as soils, sediments, and sorbents, are even more sparse. Successful remediation requires a diverse technology portfolio and a rationally designed treatment train process to overcome challenges from the complex matrices. Project 2 aims to substantially advance the mechanistic understanding and engineering performance of three promising technologies: ultraviolet photodegradation (UV), electrochemical oxidation (EO), and piezoelectric ball milling (PBM), and their integrated systems for PFAS destruction in both aqueous and solid media. Samples will be collected from the Superfund site at the former Chanute Air Force base (Rantoul, IL), wastewater treatment plants, drinking water plants, and private wells. In particular, this project highlights the identification, enrichment, and characterization of recalcitrant transformation products (TPs) of PFAS. The recalcitrant TPs may still contain a few C−F bonds and may show higher or lower toxicities than their parent PFAS. We will provide TPs from model PFAS and treatment residues from real polluted samples to the two biomedical projects to understand the effect of engineering treatment on toxicity reduction and carcinogenesis. We will advance TP characterization and minimize toxicity effects for PFAS destruction.

Select PFAS publications:

2024

  1. Liu, Z., Jin, B., Rao, D., Bentel, M., Liu, T., Gao, J., Men, Y., Liu, J.*, Oxidative transformation of Nafion-related fluorinated ether sulfonates: Comparison with legacy PFAS structures and opportunities of acidic persulfate digestion for PFAS precursor analysis. 2024.  Environmental Science & Technology, 58(14): 6415-6424.  https://doi.org/10.1021/acs.est.3c06289.
  2. Wang, Y., Zhang, J., Zhang, W., Yao, J., Liu, J., He, H., Gu, C., Gao, G.*, Jin, X. Electrostatic field in contact-electro-catalysis driven c-f bond cleavage of perfluoroalkyl substances. Angewandte Chemie 2024, e202402440. https://doi.org/10.1002/anie.202402440.
  3. Guan, Y., Liu Z., Yang, N., Yang, S., Quispe Cardenas, L. E., Liu J.*, Yang, Y.* Near-Complete Destruction of PFAS in Aqueous Film-Forming Foam (AFFF) by Integrated Photo-Electrochemical Processes. Nature Water. 2024 (Accepted)
  4. Rao, D., and Liu, J.*, Photochemical PFAS degradation in ion exchange resin regeneration brine: Effects of water matrix components and technical solutions. ChemRxiv 2024, DOI: 10.26434/chemrxiv-2024-h4bsz
  5. Rao, D.; Liu, J.*, Pretreatment methods for accelerated PFAS degradation in wastewater. ChemRxiv 2024, DOI: 10.26434/chemrxiv-2024-pqr4n

 

2023

  1. Yang N, Yang S, Ma Q, Beltran C, Guan Y, Morsey M, Brown E, Fernando S, Holsen TM, Zhang W, Yang Y. Solvent-Free Nonthermal Destruction of PFAS Chemicals and PFAS in Sediment by Piezoelectric Ball Milling. Environmental Science & Technology Letters. 2023;10(2):198-203. doi: 10.1021/acs.estlett.2c00902.
  2. Chen Z, Zhang S, Wang X, Mi N, Zhang M, Zeng G, Dong H, Liu J, Wu B, Wei S, Gu C. Amine-Functionalized A-Center Sphalerite for Selective and Efficient Destruction of Perfluorooctanoic Acid. Environmental Science & Technology. 2023;57(28):10438-47. doi: 10.1021/acs.est.3c01266.
  3. Jin B, Zhu Y, Zhao W, Liu Z, Che S, Chen K, Lin Y-H, Liu J, Men Y. Aerobic Biotransformation and Defluorination of Fluoroalkylether Substances (ether PFAS): Substrate Specificity, Pathways, and Applications. Environmental Science & Technology Letters. 2023;10(9):755-61. doi: 10.1021/acs.estlett.3c00411.
  4. Jin B, Liu H, Che S, Gao J, Yu Y, Liu J, Men Y. Substantial defluorination of polychlorofluorocarboxylic acids triggered by anaerobic microbial hydrolytic dechlorination. Nature Water. 2023;1(5):451-61. doi: 10.1038/s44221-023-00077-6.
  5. Gao J, Liu Z, Chen Z, Rao D, Che S, Gu C, Men Y, Huang J, Liu J. Photochemical degradation pathways and near-complete defluorination of chlorinated polyfluoroalkyl substances. Nature Water. 2023;1(4):381-90. doi: 10.1038/s44221-023-00046-z.

 

2022

  1. Liu Z, Chen Z, Gao J, Yu Y, Men Y, Gu C, Liu J. Accelerated Degradation of Perfluorosulfonates and Perfluorocarboxylates by UV/Sulfite + Iodide: Reaction Mechanisms and System Efficiencies. Environmental Science & Technology. 2022;56(6):3699-709. doi: 10.1021/acs.est.1c07608.
  2. Yu Y, Che S, Ren C, Jin B, Tian Z, Liu J, Men Y. Microbial Defluorination of Unsaturated Per- and Polyfluorinated Carboxylic Acids under Anaerobic and Aerobic Conditions: A Structure Specificity Study. Environmental Science & Technology. 2022;56(8):4894-904. doi: 10.1021/acs.est.1c05509.

 

2021

  1. Che S, Jin B, Liu Z, Yu Y, Liu J, Men Y. Structure-Specific Aerobic Defluorination of Short-Chain Fluorinated Carboxylic Acids by Activated Sludge Communities. Environmental Science & Technology Letters. 2021;8(8):668-74. doi: 10.1021/acs.estlett.1c00511.
  2. Cheng Z, Chen Q, Liu Z, Liu J, Liu Y, Liu S, Gao X, Tan Y, Shen Z. Interpretation of Reductive PFAS Defluorination with Quantum Chemical Parameters. Environmental Science & Technology Letters. 2021;8(8):645-50. doi: 10.1021/acs.estlett.1c00403.
  3. Gao J, Liu Z, Bentel MJ, Yu Y, Men Y, Liu J. Defluorination of Omega-Hydroperfluorocarboxylates (ω-HPFCAs): Distinct Reactivities from Perfluoro and Fluorotelomeric Carboxylates. Environmental Science & Technology. 2021;55(20):14146-55. doi: 10.1021/acs.est.1c04429.
  4. Liu Z, Bentel MJ, Yu Y, Ren C, Gao J, Pulikkal VF, Sun M, Men Y, Liu J. Near-Quantitative Defluorination of Perfluorinated and Fluorotelomer Carboxylates and Sulfonates with Integrated Oxidation and Reduction. Environmental Science & Technology. 2021;55(10):7052-62. doi: 10.1021/acs.est.1c00353.

 

2020

  1. Bentel MJ, Liu Z, Yu Y, Gao J, Men Y, Liu J. Enhanced Degradation of Perfluorocarboxylic Acids (PFCAs) by UV/Sulfite Treatment: Reaction Mechanisms and System Efficiencies at pH 12. Environmental Science & Technology Letters. 2020;7(5):351-7. doi: 10.1021/acs.estlett.0c00236.
  2. Zhuo Q, Wang J, Niu J, Yang B, Yang Y. Electrochemical oxidation of perfluorooctane sulfonate (PFOS) substitute by modified boron doped diamond (BDD) anodes. Chemical Engineering Journal. 2020;379:122280. doi: https://doi.org/10.1016/j.cej.2019.122280.
  3. Bentel MJ, Yu Y, Xu L, Kwon H, Li Z, Wong BM, Men Y, Liu J. Degradation of Perfluoroalkyl Ether Carboxylic Acids with Hydrated Electrons: Structure–Reactivity Relationships and Environmental Implications. Environmental Science & Technology. 2020;54(4):2489-99. doi: 10.1021/acs.est.9b05869.
  4. Tenorio R, Liu J, Xiao X, Maizel A, Higgins CP, Schaefer CE, Strathmann TJ. Destruction of Per- and Polyfluoroalkyl Substances (PFASs) in Aqueous Film-Forming Foam (AFFF) with UV-Sulfite Photoreductive Treatment. Environmental Science & Technology. 2020;54(11):6957-67. doi: 10.1021/acs.est.0c00961.
  5. Yu Y, Zhang K, Li Z, Ren C, Chen J, Lin Y-H, Liu J, Men Y. Microbial Cleavage of C–F Bonds in Two C6 Per- and Polyfluorinated Compounds via Reductive Defluorination. Environmental Science & Technology. 2020;54(22):14393-402. doi: 10.1021/acs.est.0c04483.
  6. Dasgupta S, Reddam A, Liu Z, Liu J, Volz DC. High-content screening in zebrafish identifies perfluorooctanesulfonamide as a potent developmental toxicant. Environmental Pollution. 2020;256:113550. doi: https://doi.org/10.1016/j.envpol.2019.113550.

 

2019

  1. Bentel MJ, Yu Y, Xu L, Li Z, Wong BM, Men Y, Liu J. Defluorination of Per- and Polyfluoroalkyl Substances (PFASs) with Hydrated Electrons: Structural Dependence and Implications to PFAS Remediation and Management. Environmental Science & Technology. 2019;53(7):3718-28. doi: 10.1021/acs.est.8b06648.
  2. Yang S, Fernando S, Holsen TM, Yang Y. Inhibition of Perchlorate Formation during the Electrochemical Oxidation of Perfluoroalkyl Acid in Groundwater. Environmental Science & Technology Letters. 2019;6(12):775-80. doi: 10.1021/acs.estlett.9b00653.

 

2018

  1. Liu J, Van Hoomissen DJ, Liu T, Maizel A, Huo X, Fernández SR, Ren C, Xiao X, Fang Y, Schaefer CE, Higgins CP, Vyas S, Strathmann TJ. Reductive Defluorination of Branched Per- and Polyfluoroalkyl Substances with Cobalt Complex Catalysts. Environmental Science & Technology Letters. 2018;5(5):289-94. doi: 10.1021/acs.estlett.8b00122.

 

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