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Frontiers of Environmental Science & Engineering

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Front. Environ. Sci. Eng.    2022, Vol. 16 Issue (5) : 55    https://doi.org/10.1007/s11783-021-1489-0
RESEARCH ARTICLE
Toward better understanding vacuum ultraviolet–iodide induced photolysis via hydrogen peroxide formation, iodine species change, and difluoroacetic acid degradation
Yang Yang, Qi Zhang, Baiyang Chen(), Liangchen Long, Guan Zhang
State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology (Shenzhen), Shenzhen 518055, China
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Abstract

• UV/VUV/I– induces substantial H2O2 and IO3– formation, but UV/I– does not.

• Increasing DO level in water enhances H2O2 and iodate productions.

• Increasing pH decreases H2O2 and iodate formation and also photo-oxidation.

• The redox potentials of UV/VUV/I– and UV/VUV changes with pH changes.

• The treatability of the UV/VUV/I– process was stronger than UV/VUV at pH 11.0.

Recently, a photochemical process induced by ultraviolet (UV), vacuum UV (VUV), and iodide (I–) has gained attention for its robust potential for contaminant degradation. However, the mechanisms behind this process remain unclear because both oxidizing and reducing reactants are likely generated. To better understand this process, this study examined the evolutions of hydrogen peroxide (H2O2) and iodine species (i.e., iodide, iodate, and triiodide) during the UV/VUV/I– process under varying pH and dissolved oxygen (DO) conditions. Results show that increasing DO in water enhanced H2O2 and iodate production, suggesting that high DO favors the formation of oxidizing species. In contrast, increasing pH (from 6.0 to 11.0) resulted in lower H2O2 and iodate formation, indicating that there was a decrease of oxidative capacity for the UV/VUV/I– process. In addition, difluoroacetic acid (DFAA) was used as an exemplar contaminant to verify above observations. Although its degradation kinetics did not follow a constant trend as pH increases, the relative importance of mineralization appeared declining, suggesting that there was a redox transition from an oxidizing environment to a reducing environment as pH rises. The treatability of the UV/VUV/I– process was stronger than UV/VUV under pH of 11.0, while UV/VUV process presented a better performance at pH lower than 11.0.
Keywords Vacuum ultraviolet      Hydrogen peroxide      Iodate      Hydroxyl radical      Redox transition     
Corresponding Author(s): Baiyang Chen   
Issue Date: 27 July 2021
 Cite this article:   
Yang Yang,Qi Zhang,Baiyang Chen, et al. Toward better understanding vacuum ultraviolet–iodide induced photolysis via hydrogen peroxide formation, iodine species change, and difluoroacetic acid degradation[J]. Front. Environ. Sci. Eng., 2022, 16(5): 55.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-021-1489-0
https://academic.hep.com.cn/fese/EN/Y2022/V16/I5/55
Equations Rate constants Ref.
(1) H2O+ hν185 → •OH+ •H Φ•OH = 0.33 Gonzalez et al., 2004
(2) H2O+ hν185 → •OH+ H+ + eaq– Φeaq– = 0.045 Gonzalez et al., 2004
(3) I– + H2O+ hν254 → I–H2O* Yeo and Choi, 2009
(4) I–H2O* → (I•, e–) + H2O Yeo and Choi, 2009
(5) (I•, e–) → I• + eaq– Φeaq– = 0.3–0.4 Qu et al., 2010
(6) (I•, e–) + O2 → I• + O2•– Yeo and Choi, 2009
(7) I• + I• → I2 k7 = 1.0 × 1010 M−1 s−1 Yeo and Choi, 2009
(8) I• + I– ↔ I2– k8>1.2 × 104 M−1 s−1 Yeo and Choi, 2009
(9) I2– + I2– → I3– + I– k9 = 3.2 × 109 M−1 s−1 Yeo and Choi, 2009
(10) I2 + I–↔ I3– k10 = 700 M−1 s−1 Yeo and Choi, 2009
(11) H2O2 ↔ H+ + HO2– pKa = 11.6 Song et al., 2017
(12) •OH ↔ H+ + •O– pKa = 11.9 Nosaka and Nosaka, 2017
(13) HO2• ↔ H+ + O2•– pKa = 4.8 Nosaka and Nosaka, 2017
(14) •H ↔ H+ + eaq– pKa = 9.7 Nosaka and Nosaka, 2017
(15) HO3• ↔ H+ + O3•– pKa = 8.2 Nosaka and Nosaka, 2017
(16) eaq– + H+ → •H k16 = 2.3 × 1010 M−1 s−1 Cui et al., 2020
(17) eaq– + •H+ H2O → H2 + OH– k17 = 3.0 × 1010 M−1 s−1 Cui et al., 2020
(18) eaq– + O2 → O2•– k18 = 1.9 × 1010 M−1 s−1 Cui et al., 2020
(19) eaq– + O2•– → O2– k19 = 1.3 × 1010 M−1 s−1 Cui et al., 2020
(20) HOI+ HOI → IO2– + I– + H+ Sun et al., 2017a
(21) HOI+ OI– → IO2– + I– + H+ Sun et al., 2017a
(22) HOI+ IO2– → IO3– + I– + H+ Sun et al., 2017a
(23) eaq– + I3– → I2•– + I– Sun et al., 2017a
(24) •OH+ •OH → H2O2 k24 = 4.0 × 109 M−1 s−1 Zhang et al., 2020
(25) •H+ O2 → HO2• k25 = 1.0 × 1010 M−1 s– Moussavi and Rezaei, 2017
(26) 2HO2• → H2O2 + O2 k26 = 2.0 × 1010 M−1 s−1 Moussavi and Rezaei, 2017
Tab.1  A summary of photochemical equations and rate constants involved in this study
Fig.1  A comparison of H2O2 formation and iodine species evolution between UV and UV/VUV photolysis processes ([I−]0 = 1.0 mg/L, DO= 8.5 mg/L, initial pH= 6.0 with no buffer used).
Fig.2  Effects of DO on H2O2 formation and iodine species evolution during UV/VUV photolysis ([I–]0 = 1.0 mg/L, initial pH= 6.0 with no buffer used).
Fig.3  Effects of pH on H2O2 formation and iodine evolution during UV/VUV photolysis ([I–]0 = 1.0 mg/L, DO= 8.5 mg/L with no buffer used).
Fig.4  A schematic of H2O2 formation and iodine species evolution during the UV/VUV/I–process.
Fig.5  Effects of pH on the rate constants of degradation (kd), mineralization (km), and defluorination (kf) of DFAA (a) and the ratio changes of km/kd, kf/kd, and kf/km (b) ([I?−]0 = 1.0 mg/L, DO= 8.5 mg/L with no buffer used).
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