Extremely Efficient Decomposition of Ammonia N to N2 Using ClO from Reactions of HO and HOCl Generated in Situ on a Novel Bifacial Photoelectroanode

  • Yan Zhang
    Yan Zhang
    School of Environmental Science and Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, People’s Republic of China
    More by Yan Zhang
  • Jinhua Li
    Jinhua Li
    School of Environmental Science and Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, People’s Republic of China
    More by Jinhua Li
  • Jing Bai*
    Jing Bai
    School of Environmental Science and Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, People’s Republic of China
    *Telephone/Fax: +86-21-54747351. E-mail: [email protected]
    More by Jing Bai
  • Linsen Li
    Linsen Li
    School of Environmental Science and Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, People’s Republic of China
    More by Linsen Li
  • Shuai Chen
    Shuai Chen
    School of Environmental Science and Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, People’s Republic of China
    More by Shuai Chen
  • Tingsheng Zhou
    Tingsheng Zhou
    School of Environmental Science and Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, People’s Republic of China
  • Jiachen Wang
    Jiachen Wang
    School of Environmental Science and Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, People’s Republic of China
    More by Jiachen Wang
  • Ligang Xia
    Ligang Xia
    College of Environmental and Chemical Engineering, Shanghai University of Electric Power, 2588 Changyang Road, Shanghai 200090, People’s Republic of China
    More by Ligang Xia
  • Qunjie Xu
    Qunjie Xu
    College of Environmental and Chemical Engineering, Shanghai University of Electric Power, 2588 Changyang Road, Shanghai 200090, People’s Republic of China
    Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, People’s Republic of China
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  • , and 
  • Baoxue Zhou*
    Baoxue Zhou
    School of Environmental Science and Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, People’s Republic of China
    Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, People’s Republic of China
    Key Laboratory of Thin Film and Microfabrication Technology, Ministry of Education, Shanghai 200240, People’s Republic of China
    *Telephone/Fax: +86-21-54747351. E-mail: [email protected]
    More by Baoxue Zhou
Cite this: Environ. Sci. Technol. 2019, 53, 12, 6945–6953
Publication Date (Web):May 22, 2019
https://doi.org/10.1021/acs.est.9b00959
Copyright © 2019 American Chemical Society
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Abstract

The conversion of excess ammonia N into harmless N2 is a primary challenge for wastewater treatment. We present here a method to generate ClO directionally for quick and efficient decomposition of NH4+ N to N2. ClO was produced and enhanced by a bifacial anode, a front WO3 photoanode and a rear Sb–SnO2 anode, in which HO generated on WO3 reacts with HClO generated on Sb–SnO2 to form ClO. Results show that the ammonia decomposition rate of Sb–SnO2/WO3 is 4.4 times than that of WO3 and 3.3 times than that of Sb–SnO2, with achievement of the removal of NH4+ N on Sb–SnO2/WO3 and WO3 being 99.2 and 58.3% in 90 min, respectively. This enhancement is attributed to the high rate constant of ClO with NH4+ N, which is 2.8 and 34.8 times than those of Cl and HO, respectively. The steady-state concentration of ClO (2.5 × 10–13 M) is 102 times those of HO and Cl, and this is further confirmed by kinetic simulations. In combination with the Pd–Cu/NF cathode to form a denitrification exhaustion system, Sb–SnO2/WO3 shows excellent total nitrogen removal (98.4%), which is more effective than WO3 (47.1%) in 90 min. This study provides new insight on the directed ClO generation and its application on ammonia wastewater treatment.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.9b00959.

  • Description of the preparation of the WO3 photoanode and analytical methods of NB, BA, and DMOB, SEM, XRD, and LSV measurements of the Sb–SnO2/WO3 photoanode, model simulation results, second-order rate constants of NH4+ reacting with ClO, Cl, and OH, degradation of NH4+ N by HClO in the presence of WO3, removal of NH4+ N under different pH, applied potential, Sb–SnO2 layers, and NH4+ N initial concentration, time profiles of ClO3 ions, current efficiency and energy consumption, stability test of Sb–SnO2/WO3, performance of Sb–SnO2/WO3 for degrading real wastewater, total nitrogen removal mechanism and performance in the exhaustive denitrification system, details of the kinetic model, rate constants of scavengers reacting with different radicals, and actual wastewater composition (PDF)

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