Electrochemical Oxidation of Atrazine and Clothianidin on Bi-doped SnO2–TinO2n–1 Electrocatalytic Reactive Electrochemical Membranes

  • Pralay Gayen
    Pralay Gayen
    Department of Chemical Engineering, University of Illinois at Chicago, 810 S. Clinton St., Chicago, Illinois 60607, United States
    More by Pralay Gayen
  • Chen Chen
    Chen Chen
    Department of Mechanical and Industrial Engineering, University of Illinois at Chicago, 842 W. Taylor St., Chicago, Illinois 60607, United States
    More by Chen Chen
  • Jeremiah T. Abiade
    Jeremiah T. Abiade
    Department of Mechanical and Industrial Engineering, University of Illinois at Chicago, 842 W. Taylor St., Chicago, Illinois 60607, United States
  • , and 
  • Brian P. Chaplin*
    Brian P. Chaplin
    Department of Chemical Engineering, University of Illinois at Chicago, 810 S. Clinton St., Chicago, Illinois 60607, United States
    *Phone: +13129960288. E-mail: [email protected]
Cite this: Environ. Sci. Technol. 2018, 52, 21, 12675–12684
Publication Date (Web):September 21, 2018
https://doi.org/10.1021/acs.est.8b04103
Copyright © 2018 American Chemical Society
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Abstract

This research focused on improving mineralization rates during the advanced electrochemical oxidation treatment of agricultural water contaminants. For the first time, bismuth-doped tin oxide (BDTO) catalysts were deposited on Magnéli phase (TinO2n–1, n = 4–6) reactive electrochemical membranes (REMs). Terephthalic acid (TA) was used as a OH probe, whereas atrazine (ATZ) and clothianidin (CDN) were chosen as model agricultural water contaminants. The BDTO-deposited REMs (REM/BDTO) showed higher compound removal than the REM, due to enhanced OH production. At 3.5 V/SHE, complete mineralization of TA, ATZ, and CDN was achieved for the REM/BDTO upon a single pass in the reactor (residence time ∼3.6 s). Energy consumption for REM/BDTO was as much as 31-fold lower than the REM, with minimal values per log removal of <0.53 kWh m–3 for TA (3.5 V/SHE), <0.42 kWh m–3 for ATZ (3.0 V/SHE), and 0.83 kWh m–3 for CDN (3.0 V/SHE). Density functional theory simulations provided potential dependent activation energy profiles for ATZ, CDN, and various oxidation products. Efficient mass transfer and a reaction mechanism involving direct electron transfer and reaction with OH were responsible for the rapid and complete mineralization of ATZ and CDN at very short residence times.

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