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Front. Environ. Sci. Eng.    2020, Vol. 14 Issue (2) : 34    https://doi.org/10.1007/s11783-019-1213-5
RESEARCH ARTICLE
Zero-valent manganese nanoparticles coupled with different strong oxidants for thallium removal from wastewater
Keke Li1, Huosheng Li2(), Tangfu Xiao1, Gaosheng Zhang1, Aiping Liang1, Ping Zhang3, Lianhua Lin1, Zexin Chen1, Xinyu Cao1, Jianyou Long1()
1. School of Environmental Science and Engineering, Guangzhou University, Guangzhou 510006, China
2. Institute of Environmental Research at Greater Bay Area, Key Laboratory for Water Quality and Conservation of Pearl River Delta (Ministry of Education), Guangzhou University, Guangzhou 510006, China
3. School of Chemistry and Chemical Engineering, Guangzhou University, Guangzhou 510006, China
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Abstract

• Nano zero-valent manganese (nZVMn, Mn0) is synthesized via borohydrides reduction.

• Mn0 combined with persulfate/hypochlorite is effective for Tl removal at pH 6-12.

• Mn0 can activate persulfate to form hydroxyl and sulfate radicals.

• Oxidation-induced precipitation and surface complexation contribute to Tl removal.

• Combined Mn0-oxidants process is promising in the environmental field.

Nano zero-valent manganese (nZVMn, Mn0) was prepared through a borohydride reduction method and coupled with different oxidants (persulfate (S2O82−), hypochlorite (ClO−), or hydrogen peroxide (H2O2)) to remove thallium (Tl) from wastewater. The surface of Mn0 was readily oxidized to form a core-shell composite (MnOx@Mn0), which consists of Mn0 as the inner core and MnOx (MnO, Mn2O3, and Mn3O4) as the outer layer. When Mn0 was added alone, effective Tl(I) removal was achieved at high pH levels (>12). The Mn0-H2O2 system was only effective in Tl(I) removal at high pH (>12), while the Mn0-S2O82− or Mn0-ClO− system had excellent Tl(I) removal (>96%) over a broad pH range (4–12). The Mn0-S2O82− oxidation system provided the best resistance to interference from an external organic matrix. The isotherm of Tl(I) removal through the Mn0-S2O82− system followed the Freundlich model. The Mn0 nanomaterials can activate persulfate to produce sulfate radicals and hydroxyl radicals. Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy suggested that oxidation-induced precipitation, surface adsorption, and electrostatic attraction are the main mechanisms for Tl(I) removal resulting from the combination of Mn0 and oxidants. Mn0 coupled with S2O82−/ClO− is a novel and effective technique for Tl(I) removal, and its application in other fields is worthy of further investigation.
Keywords Nano zero-valent manganese      Thallium      Adsorption      Oxidation      Sulfate radical      Hydroxyl radical     
Corresponding Author(s): Huosheng Li,Jianyou Long   
Issue Date: 11 February 2020
 Cite this article:   
Keke Li,Huosheng Li,Tangfu Xiao, et al. Zero-valent manganese nanoparticles coupled with different strong oxidants for thallium removal from wastewater[J]. Front. Environ. Sci. Eng., 2020, 14(2): 34.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-019-1213-5
https://academic.hep.com.cn/fese/EN/Y2020/V14/I2/34
Fig.1  Characterization of the as-prepared Mn0 nanoparticles: (a, b) TEM images, (c) selective area electron diffraction image, (d) high-resolution TEM image, (e) XRD patterns, and (f) particle size distribution.
Fig.2  Factors  influencing Tl(I) removal: (a) initial pH, (b) coagulation pH, (c) oxidant dosage without adsorbent; (d) oxidant dosage with 2 g/L Mn0 (Tl(I)0 = 10 mg/L, Mn0 dosage= 2 g/L, and reaction time= 30 min; for (a) and (b), if present, Na2S2O8 = 6 g/L, ClO- = 40 mmol/L, H2O2 = 40 mmol/L; for (c) and (d), initial pH= 10, coagulation pH= 10).
Fig.3  Influence of (a)  co-existing organics and (b) cations on Tl(I) removal: (Tl(I)0 = 10 mg/L, Mn0 dosage= 2 g/L, initial pH= 10, coagulation pH= 10, and reaction time= 30 min; if present, Na2S2O8 = 6 g/L, ClO- = 40 mmol/L, H2O2 = 40 mmol/L).
Fig.4  Isotherms of  Tl(I) removal using the Mn0-S2O82- system (initial pH= 10, coagulation pH= 10, Tl(I)0 = 10–500 mg/L, Mn0 dosage= 2 g/L, Na2S2O8 = 6 g/L, and reaction time= 30 min).
Fig.5  XPS spectra of  the Mn0 before and after adsorption of Tl: (a) survey, (b) Mn 2p, (c) O 1s, (d) Tl 4f.
Fig.6  ESR spectra of  the free oxygenous radicals captured by DMPO.
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