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Ferrate self-decomposition in water is also a self-activation process: Role of Fe(V) species and enhancement with Fe(III) in methyl phenyl sulfoxide oxidation by excess ferrate.
Water Res. 2021 Jun 01; 197:117094.WR

Abstract

To reveal the role of ferrate self-decomposition and the fates of intermediate iron species [Fe(V)/Fe(IV) species] during ferrate oxidation, the reaction between ferrate and methyl phenyl sulfoxide (PMSO) at pH 7.0 was investigated as a model system in this study. Interestingly, the apparent second-order rate constants (kapp) between ferrate and PMSO was found to increase with ferrate dosage in the condition of excess ferrate in borate buffer. This ferrate dosage effect was diminished greatly in the condition of excess PMSO where ferrate self-decomposition was lessened largely, or counterbalanced by adding a strong complexing ligand (e.g. pyrophosphate) to sequester Fe(V) oxidation, demonstrating that the Fe(V) species derived from ferrate self-decomposition plays an important role in PMSO oxidation. A mechanistic kinetics model involving the ferrate self-decomposition and PMSO oxidation by Fe(VI), Fe(V) and Fe(IV) species was then developed and validated. The modeling results show that up to 99% of the PMSO oxidation was contributed by the ferrate self-decomposition resultant Fe(V) species in borate buffer, revealing that ferrate self-decomposition is also a self-activation process. The direct Fe(VI) oxidation of PMSO was impervious to presence of phosphate or Fe(III), while the Fe(V) oxidation pathway was strongly inhibited by phosphate complexation or enhanced with Fe(III). Similar ferrate dosage effect and its counterbalance by pyrophosphate as well as the Fe(III) enhancement were also observed in ferrate oxidation of micropollutants like carbamazepine, diclofenac and sulfamethoxazole, implying the general role of Fe(V) and promising Fe(III) enhancement during ferrate oxidation of micropollutants.

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Publisher Full Text (DOI)

Authors+Show Affiliations

State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China.

State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China. Electronic address: wanglu9195@163.com.

State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China.

State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China.

State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China.

Civil Engineering, College of Engineering and Informatics, National University of Ireland, Galway, Ireland.

State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China.

MeSH

Ferric CompoundsIronKineticsOxidation-ReductionSulfoxidesWaterWater Pollutants, ChemicalWater Purification

Pub Type(s)

Journal Article

Language

eng

PubMed ID

33836297

Citation

Huang, Zhuang-Song, et al. "Ferrate Self-decomposition in Water Is Also a Self-activation Process: Role of Fe(V) Species and Enhancement With Fe(III) in Methyl Phenyl Sulfoxide Oxidation By Excess Ferrate." Water Research, vol. 197, 2021, p. 117094.

Huang ZS, Wang L, Liu YL, et al. Ferrate self-decomposition in water is also a self-activation process: Role of Fe(V) species and enhancement with Fe(III) in methyl phenyl sulfoxide oxidation by excess ferrate. Water Res. 2021;197:117094.

Huang, Z. S., Wang, L., Liu, Y. L., Zhang, H. Y., Zhao, X. N., Bai, Y., & Ma, J. (2021). Ferrate self-decomposition in water is also a self-activation process: Role of Fe(V) species and enhancement with Fe(III) in methyl phenyl sulfoxide oxidation by excess ferrate. Water Research, 197, 117094. https://doi.org/10.1016/j.watres.2021.117094

Huang ZS, et al. Ferrate Self-decomposition in Water Is Also a Self-activation Process: Role of Fe(V) Species and Enhancement With Fe(III) in Methyl Phenyl Sulfoxide Oxidation By Excess Ferrate. Water Res. 2021 Jun 1;197:117094. PubMed PMID: 33836297.

* Article titles in AMA citation format should be in sentence-case

TY - JOUR T1 - Ferrate self-decomposition in water is also a self-activation process: Role of Fe(V) species and enhancement with Fe(III) in methyl phenyl sulfoxide oxidation by excess ferrate. AU - Huang,Zhuang-Song, AU - Wang,Lu, AU - Liu,Yu-Lei, AU - Zhang,Hong-Yan, AU - Zhao,Xiao-Na, AU - Bai,Yang, AU - Ma,Jun, Y1 - 2021/03/29/ PY - 2020/12/27/received PY - 2021/03/22/revised PY - 2021/03/25/accepted PY - 2021/4/10/pubmed PY - 2021/4/30/medline PY - 2021/4/9/entrez KW - Ferrate KW - Intermediate iron species KW - Kinetics KW - Micropollutants KW - Oxidation SP - 117094 EP - 117094 JF - Water research JO - Water Res VL - 197 N2 - To reveal the role of ferrate self-decomposition and the fates of intermediate iron species [Fe(V)/Fe(IV) species] during ferrate oxidation, the reaction between ferrate and methyl phenyl sulfoxide (PMSO) at pH 7.0 was investigated as a model system in this study. Interestingly, the apparent second-order rate constants (kapp) between ferrate and PMSO was found to increase with ferrate dosage in the condition of excess ferrate in borate buffer. This ferrate dosage effect was diminished greatly in the condition of excess PMSO where ferrate self-decomposition was lessened largely, or counterbalanced by adding a strong complexing ligand (e.g. pyrophosphate) to sequester Fe(V) oxidation, demonstrating that the Fe(V) species derived from ferrate self-decomposition plays an important role in PMSO oxidation. A mechanistic kinetics model involving the ferrate self-decomposition and PMSO oxidation by Fe(VI), Fe(V) and Fe(IV) species was then developed and validated. The modeling results show that up to 99% of the PMSO oxidation was contributed by the ferrate self-decomposition resultant Fe(V) species in borate buffer, revealing that ferrate self-decomposition is also a self-activation process. The direct Fe(VI) oxidation of PMSO was impervious to presence of phosphate or Fe(III), while the Fe(V) oxidation pathway was strongly inhibited by phosphate complexation or enhanced with Fe(III). Similar ferrate dosage effect and its counterbalance by pyrophosphate as well as the Fe(III) enhancement were also observed in ferrate oxidation of micropollutants like carbamazepine, diclofenac and sulfamethoxazole, implying the general role of Fe(V) and promising Fe(III) enhancement during ferrate oxidation of micropollutants. SN - 1879-2448 UR - https://www.unboundmedicine.com/medline/citation/33836297/Ferrate_self_decomposition_in_water_is_also_a_self_activation_process:_Role_of_Fe_V__species_and_enhancement_with_Fe_III__in_methyl_phenyl_sulfoxide_oxidation_by_excess_ferrate_ DB - PRIME DP - Unbound Medicine ER -