C3N4–Mn/CNT composite as a heterogeneous catalyst in the electro-peroxone process for promoting the reaction between O3 and H2O2 in acid solution

The electro-peroxone (E-P) process normally exhibits low efficiency in organic degradation in acid solution due to the limited rate constant of the reaction between O3 and H2O2 (peroxone reaction). In this paper, a C3N4–Mn/CNT composite material was synthetized and characterized with XRD, FTIR, SEM and XPS. With the function of the C3N4–Mn/CNT catalyst, the substrate oxalic acid (OA) was completely degraded in the E-P process within 30 min at pH 3, while only 15% degradation could be achieved after 60 min without the catalyst. The comparison of different reaction systems using the C3N4–Mn/CNT catalyst confirmed that the catalyst promoted the peroxone reaction, rather than the catalytic ozonation or electro-Fenton like reaction. Correlating the XRD and XPS analysis with the degradation data using the C3N4–Mn/CNT catalyst, we deduced that Mn coordinated with nitrogen was the active site for the peroxone reaction. Furthermore, the catalyst showed good chemical and catalytic stability in five cycles of the E-P process for OA degradation.

[1]  Jun Huang,et al.  The electro-peroxone process for the abatement of emerging contaminants: Mechanisms, recent advances, and prospects. , 2018, Chemosphere.

[2]  Yujue Wang,et al.  Pilot-scale evaluation of micropollutant abatements by conventional ozonation, UV/O3, and an electro-peroxone process. , 2018, Water research.

[3]  Hongbin Cao,et al.  High activity of g-C3N4/multiwall carbon nanotube in catalytic ozonation promotes electro-peroxone process. , 2018, Chemosphere.

[4]  Jiaguo Yu,et al.  First-principle calculation study of tri- s -triazine-based g-C 3 N 4 : A review , 2018 .

[5]  Haiping Li,et al.  Enhanced charge carrier separation of manganese(II)-doped graphitic carbon nitride: formation of N–Mn bonds through redox reactions , 2018 .

[6]  Jun Huang,et al.  Comparison of pharmaceutical abatement in various water matrices by conventional ozonation, peroxone (O3/H2O2), and an electro-peroxone process. , 2018, Water research.

[7]  Hongbin Cao,et al.  Towards a better understanding of the synergistic effect in the electro-peroxone process using a three electrode system , 2017 .

[8]  Xu Zhao,et al.  Peroxymonosulfate enhanced visible light photocatalytic degradation bisphenol A by single-atom dispersed Ag mesoporous g-C3N4 hybrid , 2017 .

[9]  Jun Huang,et al.  The competition between cathodic oxygen and ozone reduction and its role in dictating the reaction mechanisms of an electro-peroxone process. , 2017, Water research.

[10]  R. Jung,et al.  Photocatalytic improvement of Mn-adsorbed g-C3N4 , 2017 .

[11]  Weiqi Wang,et al.  Effective degradation of diatrizoate by electro-peroxone process using ferrite/carbon nanotubes based gas diffusion cathode , 2017 .

[12]  Hongbin Cao,et al.  Enhanced hole-dominated photocatalytic activity of doughnut-like porous g-C3N4 driven by down-shifted valance band maximum , 2017, Catalysis Today.

[13]  Gang Yu,et al.  Kinetics and operational parameters for 1,4-dioxane degradation by the photoelectro-peroxone process , 2017 .

[14]  Jianqing Ma,et al.  Fe-g-C3N4/graphitized mesoporous carbon composite as an effective Fenton-like catalyst in a wide pH range , 2017 .

[15]  Yu Zhou,et al.  Electric field induced activated carbon fiber (ACF) cathode transition from an initiator/a promoter into an electrocatalyst in ozonation process , 2016 .

[16]  Hongbin Cao,et al.  Towards effective design of active nanocarbon materials for integrating visible-light photocatalysis with ozonation , 2016 .

[17]  Siang-Piao Chai,et al.  Graphitic Carbon Nitride (g-C3N4)-Based Photocatalysts for Artificial Photosynthesis and Environmental Remediation: Are We a Step Closer To Achieving Sustainability? , 2016, Chemical reviews.

[18]  Zhengguo Zhang,et al.  Constructing a novel ternary Fe(III)/graphene/g-C3N4 composite photocatalyst with enhanced visible-light driven photocatalytic activity via interfacial charge transfer effect , 2016 .

[19]  M. Tadé,et al.  Carbocatalytic activation of persulfate for removal of antibiotics in water solutions , 2016 .

[20]  Feng Duan,et al.  Super synergy between photocatalysis and ozonation using bulk g-C3N4 as catalyst: A potential sunlight/O3/g-C3N4 method for efficient water decontamination , 2016 .

[21]  Shaobin Wang,et al.  2D/2D nano-hybrids of γ-MnO₂ on reduced graphene oxide for catalytic ozonation and coupling peroxymonosulfate activation. , 2016, Journal of hazardous materials.

[22]  Jun Huang,et al.  Electro-peroxone treatment of the antidepressant venlafaxine: Operational parameters and mechanism. , 2015, Journal of hazardous materials.

[23]  P. Gai,et al.  A ternary hybrid of carbon nanotubes/graphitic carbon nitride nanosheets/gold nanoparticles used as robust substrate electrodes in enzyme biofuel cells. , 2015, Chemical communications.

[24]  Jun Huang,et al.  Mechanisms of enhanced total organic carbon elimination from oxalic acid solutions by electro-peroxone process. , 2015, Water research.

[25]  K. Artyushkova,et al.  Bio-inspired design of electrocatalysts for oxalate oxidation: a combined experimental and computational study of Mn-N-C catalysts. , 2015, Physical chemistry chemical physics : PCCP.

[26]  M. Tadé,et al.  New insights into heterogeneous generation and evolution processes of sulfate radicals for phenol degradation over one-dimensional α-MnO2 nanostructures , 2015 .

[27]  Shaozheng Hu,et al.  Enhanced visible light photocatalytic performance of g-C3N4 photocatalysts co-doped with iron and phosphorus , 2014 .

[28]  Yong Wang,et al.  Combination of carbon nitride and carbon nanotubes: synergistic catalysts for energy conversion. , 2014, ChemSusChem.

[29]  Mietek Jaroniec,et al.  Graphitic carbon nitride nanosheet-carbon nanotube three-dimensional porous composites as high-performance oxygen evolution electrocatalysts. , 2014, Angewandte Chemie.

[30]  S. Ji,et al.  Synergy among manganese, nitrogen and carbon to improve the catalytic activity for oxygen reduction reaction , 2014 .

[31]  S. Komarneni,et al.  Electro-peroxone treatment of Orange II dye wastewater. , 2013, Water research.

[32]  T. Schmidt,et al.  The (•)OH radical yield in the H2O2 + O3 (peroxone) reaction. , 2013, Environmental science & technology.

[33]  Yujue Wang,et al.  Effective degradation of refractory organic pollutants in landfill leachate by electro-peroxone treatment , 2013 .

[34]  Z. Li,et al.  Effective degradation of methylene blue by a novel electrochemically driven process , 2013 .

[35]  U. Gunten,et al.  Chemistry of Ozone in Water and Wastewater Treatment , 2012 .

[36]  F. Wei,et al.  An oxygen reduction electrocatalyst based on carbon nanotube-graphene complexes. , 2012, Nature nanotechnology.

[37]  M. Antonietti,et al.  Synthesis of transition metal-modified carbon nitride polymers for selective hydrocarbon oxidation. , 2010, ChemSusChem.

[38]  Jun Ma,et al.  Effect of ozonation pretreatment on the surface properties and catalytic activity of multi-walled carbon nanotube , 2009 .

[39]  M. Oturan,et al.  Electro-Fenton process and related electrochemical technologies based on Fenton's reaction chemistry. , 2009, Chemical reviews.

[40]  M. Antonietti,et al.  Fe-g-C3N4-catalyzed oxidation of benzene to phenol using hydrogen peroxide and visible light. , 2009, Journal of the American Chemical Society.

[41]  U. von Gunten,et al.  Characterization of Oxidation processes: ozonation and the AOP O3/H2O2 , 2001 .

[42]  Jun Ma,et al.  Degradation of atrazine by manganese-catalysed ozonation: Influence of humic substances , 1999 .

[43]  J. Hoigné,et al.  Photometric method for the determination of low concentrations of hydrogen peroxide by the peroxidase catalyzed oxidation of N,N-diethyl-p-phenylenediamine (DPD) , 1988 .

[44]  Johannes Staehelin,et al.  Decomposition of ozone in water: rate of initiation by hydroxide ions and hydrogen peroxide , 1982 .

[45]  Yujue Wang,et al.  Comparison of methylisoborneol and geosmin abatement in surface water by conventional ozonation and an electro-peroxone process. , 2017, Water research.

[46]  Jun Huang,et al.  Removal of pharmaceuticals from secondary effluents by an electro-peroxone process. , 2016, Water research.