Reactive Nitrogen Species Mediated Degradation of Estrogenic Disrupting Chemicals by Biochar/Monochloramine in Buffered Water and Synthetic Hydrolyzed Urine

  • Zijian Wang
    Zijian Wang
    School of Environmental Science and Engineering, Tianjin University, Tianjin 300072, China
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  • Peizhe Sun*
    Peizhe Sun
    School of Environmental Science and Engineering, Tianjin University, Tianjin 300072, China
    *E-mail: [email protected] (P.S.).
    More by Peizhe Sun
  • Yaxiu Li
    Yaxiu Li
    School of Environmental Science and Engineering, Tianjin University, Tianjin 300072, China
    More by Yaxiu Li
  • Tan Meng
    Tan Meng
    School of Environmental Science and Engineering, Tianjin University, Tianjin 300072, China
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  • Zhipeng Li
    Zhipeng Li
    School of Environmental Science and Engineering, Tianjin University, Tianjin 300072, China
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  • Xu Zhang
    Xu Zhang
    School of Civil Engineering, Beijing Jiaotong University, Beijing 100044, China
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  • Ruochun Zhang
    Ruochun Zhang
    Institute of Surface-Earth System Science, Tianjin University, Tianjin 300072, China
  • Hanzhong Jia*
    Hanzhong Jia
    College of Resources and Environment, Northwest A& F University, Yangling 712100, P. R. China
    *E-mail: [email protected] (H.J.).
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  • , and 
  • Hong Yao
    Hong Yao
    School of Civil Engineering, Beijing Jiaotong University, Beijing 100044, China
    More by Hong Yao
Cite this: Environ. Sci. Technol. 2019, 53, 21, 12688–12696
Publication Date (Web):October 18, 2019
https://doi.org/10.1021/acs.est.9b04704
Copyright © 2019 American Chemical Society
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Abstract

There is increasing concern about the severe endocrine-related health problems because of the discharge of estrogenic disrupting chemicals (EDCs) into the natural environment. In this study, we investigated the activation of monochloramine (NH2Cl) by biochar [pyrolyzed by cotton straw at 350 °C (Cot350), wheat straw at 350 and 700 °C (WS350 and WS700), and corn straw at 350 and 700 °C (CS350 and CS700)] for the degradation of estradiol (E2) and ethinylestradiol (EE2). Approximately 95% of parent E2 and EE2 was removed by Cot350/NH2Cl in buffered solution, and 87% of E2 and 75% of EE2 were removed in urine within 24 h. Electronic paramagnetic resonance analysis and radical-quenching experiments showed that biochar activated NH2Cl and primarily generated NO radicals for the degradation of the EDCs. The nitrogen and silicon elements of Cot350 served as primary catalytic sites for NH2Cl activation, whereas the sp2-hybridized carbon on WS700 and CS700 played a major role. The effect of major urine components (i.e., ammonia species, chloride, and bicarbonate) on the reaction pathways of biochar/NH2Cl was also elucidated. This study provides new insights into the reaction pathways of NH2Cl activation by biochar and suggests potential applications for other carbonaceous materials for NH2Cl activation.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.9b04704.

  • Chemical materials; biochar preparation; analytic methods; composition of hydrolyzed urine; molecular structure and molecular weight of targeting pollutants; characteristics of five biochar; SWCNT characterization; concentrations of PFRs, line width, and g-factors; point of zero charge of Cot350; amount of E2 and EE2 measured by HPLC; recombined estrogenic yeast plate; E2 and EE2 degradation; EDC removal; results of linear sweep voltammetry; EPR results of DMPO-PBS and DMPO; EPR spectra of suspension, spin concentrations, and FTIR spectra of five biochars; XPS results of Cot350, CS350, CS700, WS350, and WS700; and correlation analysis of the relationship between MBET, TPV, APS, and the degradation of E2 and EE2 (PDF)

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