Constructing an Acidic Microenvironment by MoS2 in Heterogeneous Fenton Reaction for Pollutant Control.

Although Fenton or Fenton-like reactions have been widely used in the environment, biology, life science and other fields, the sharp decrease in their activity under macroneutral conditions is still a large problem. This study reports a MoS2 cocatalytic heterogeneous Fenton (CoFe2O4/MoS2) system capable of sustainably degrading organic pollutants, such as phenol, in a macroneutral buffer solution. An acidic microenvironment in the slipping plane of CoFe2O4 is successfully constructed by chemically bonding with MoS2. This microenvironment is not affected by the surrounding pH, which ensures the stable circulation of Fe3+/Fe2+ on the surface of CoFe2O4/MoS2 under neutral or even alkaline conditions. Additionally, CoFe2O4/MoS2 always exposes "fresh" active sites for the decomposition of H2O2 and the generation of 1O2, effectively inhibiting the production of iron sludge and enhancing the remediation of organic pollutants, even in actual wastewater. This work not only experimentally verifies the existence of an acidic microenvironment on the surface of heterogeneous catalysts for the first time but also eliminates the pH limitation of the Fenton reaction for pollutant remediation, thereby expanding the applicability of Fenton technology.

[1]  Yi Cui,et al.  Organic wastewater treatment by a single-atom catalyst and electrolytically produced H2O2 , 2020, Nature Sustainability.

[2]  M. Xing,et al.  Tuning Redox Reactions via Defects on CoS2-x for Sustainable Degradation of Organic Pollutants. , 2020, Angewandte Chemie.

[3]  M. Xing,et al.  Designing 3D-MoS2 Sponge as Excellent Cocatalysts in Advanced Oxidation Processes for Pollutant Control. , 2020, Angewandte Chemie.

[4]  Jin Jiang,et al.  Quantitative evaluation of relative contribution of high-valent iron species and sulfate radical in Fe(VI) enhanced oxidation processes via sulfur reducing agents activation , 2020 .

[5]  J. Dai,et al.  The exchange bias effects of CoFe2O4@NiO nanofibers fabricated by electrospinning , 2020, Materials Research Express.

[6]  F. Alcaide,et al.  A highly stable MOF-engineered FeS2/C nanocatalyst for heterogeneous electro-Fenton treatment: Validation in wastewater at mild pH. , 2020, Environmental science & technology.

[7]  M. Xing,et al.  Metallic Active Sites on MoO2(110) Surface to Catalyze Advanced Oxidation Processes for Efficient Pollutant Removal , 2020, iScience.

[8]  W. Qiu,et al.  Relative contribution of ferryl ion species (Fe(IV)) and sulfate radical formed in nanoscale zero valent iron activated peroxydisulfate and peroxymonosulfate processes. , 2020, Water research.

[9]  Xuqing Li,et al.  In-situ generation of multi-homogeneous/heterogeneous Fe-based Fenton catalysts toward rapid degradation of organic pollutants at near neutral pH. , 2019, Chemosphere.

[10]  Janeth Sanabria,et al.  Photo-Fenton process at natural conditions of pH, iron, ions, and humic acids for degradation of diuron and amoxicillin , 2019, Environmental Science and Pollution Research.

[11]  M. Xing,et al.  Efficient Fe(III)/Fe(II) cycling triggered by MoO2 in Fenton reaction for the degradation of dye molecules and the reduction of Cr(VI) , 2019 .

[12]  Z. Fang,et al.  Green synthesis of Fe-based material using tea polyphenols and its application as a heterogeneous Fenton-like catalyst for the degradation of lincomycin , 2019, Journal of Cleaner Production.

[13]  M. Xing,et al.  Singlet Oxygen Triggered by Superoxide Radicals in a Molybdenum Cocatalytic Fenton Reaction with Enhanced REDOX Activity in the Environment. , 2019, Environmental science & technology.

[14]  Jinyang Chen,et al.  Recyclable Fenton-like catalyst based on zeolite Y supported ultrafine, highly-dispersed Fe2O3 nanoparticles for removal of organics under mild conditions , 2019, Chinese Chemical Letters.

[15]  M. Xing,et al.  Molybdenum sulfide Co-catalytic Fenton reaction for rapid and efficient inactivation of Escherichia coli. , 2018, Water research.

[16]  Yi Yang,et al.  Is Sulfate Radical Really Generated from Peroxydisulfate Activated by Iron(II) for Environmental Decontamination? , 2018, Environmental science & technology.

[17]  M. Xing,et al.  Metal Sulfides as Excellent Co-catalysts for H2O2 Decomposition in Advanced Oxidation Processes , 2018, Chem.

[18]  Chao Yang,et al.  Oxygen Vacancy Promoted Heterogeneous Fenton-like Degradation of Ofloxacin at pH 3.2-9.0 by Cu Substituted Magnetic Fe3O4@FeOOH Nanocomposite. , 2017, Environmental science & technology.

[19]  Ning Xue,et al.  Composite of Few-Layered MoS2 Grown on Carbon Black: Tuning the Ratio of Terminal to Total Sulfur in MoS2 for Hydrogen Evolution Reaction , 2017 .

[20]  Tae Whan Kim,et al.  Enhanced field emission properties of molybdenum disulphide few layer nanosheets synthesized by hydrothermal method , 2016 .

[21]  M. Cecchini,et al.  Ultrastructural Characterization of the Lower Motor System in a Mouse Model of Krabbe Disease , 2016, Scientific Reports.

[22]  M. Pal,et al.  Synthesis of pyrite FeS2 nanorods by simple hydrothermal method and its photocatalytic activity , 2016 .

[23]  D. Errandonea,et al.  Cobalt ferrite nanoparticles under high pressure , 2015 .

[24]  Kun Chen,et al.  Application of response surface methodology for optimization of Orange II removal by heterogeneous Fenton-like process using Fe3O4 nanoparticles , 2014 .

[25]  M. Koinuma,et al.  Sulfurized limonite as material for fast decomposition of organic compounds by heterogeneous Fenton reaction. , 2014, Journal of hazardous materials.

[26]  Niall McEvoy,et al.  Edge and confinement effects allow in situ measurement of size and thickness of liquid-exfoliated nanosheets , 2014, Nature Communications.

[27]  Jinhua Ye,et al.  MoS2/graphene cocatalyst for efficient photocatalytic H2 evolution under visible light irradiation. , 2014, ACS nano.

[28]  G. Rajaraman,et al.  Mechanistic insights on the ortho-hydroxylation of aromatic compounds by non-heme iron complex: a computational case study on the comparative oxidative ability of ferric-hydroperoxo and high-valent Fe(IV)═O and Fe(V)═O intermediates. , 2013, Journal of the American Chemical Society.

[29]  C. Chen,et al.  A highly active bimetallic oxides catalyst supported on Al-containing MCM-41 for Fenton oxidation of phenol solution , 2011 .

[30]  S. Fukuzumi,et al.  Metal ion effect on the switch of mechanism from direct oxygen transfer to metal ion-coupled electron transfer in the sulfoxidation of thioanisoles by a non-heme iron(IV)-oxo complex. , 2011, Journal of the American Chemical Society.

[31]  Keyan Li,et al.  Estimation of electronegativity values of elements in different valence states. , 2006, The journal of physical chemistry. A.

[32]  A. Bakac,et al.  Aqueous FeIV==O: spectroscopic identification and oxo-group exchange. , 2005, Angewandte Chemie.

[33]  F. Carrasco-Marín,et al.  Activated Carbon Surface Modifications by Nitric Acid, Hydrogen Peroxide, and Ammonium Peroxydisulfate Treatments , 1995 .

[34]  S. Linn,et al.  Toxic DNA damage by hydrogen peroxide through the Fenton reaction in vivo and in vitro. , 1988, Science.

[35]  Jun Ma,et al.  Oxidation of sulfoxides and arsenic(III) in corrosion of nanoscale zero valent iron by oxygen: evidence against ferryl ions (Fe(IV)) as active intermediates in Fenton reaction. , 2011, Environmental science & technology.