Ultrafine ZnCo2O4 QD-incorporated carbon nitride mediated peroxymonosulfate activation for norfloxacin oxidation: performance, mechanisms and pathways

Recently, peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) are being actively investigated as a potential technology for water decontamination and many efforts have been made to improve the activation efficiency of PMS. Herein, a 0D metal oxide quantum dot (QD)–2D ultrathin g-C3N4 nanosheet (ZnCo2O4/g-C3N4) hybrid was facilely fabricated through a one-pot hydrothermal process and used as an efficient PMS activator. Benefiting from the restricted growth effect of the g-C3N4 support, ultrafine ZnCo2O4 QDs (∼3–5 nm) are uniformly and stably anchored onto the surface. The ultrafine ZnCo2O4 possesses high specific surface areas and shortened mass/electron transport route so that the internal static electric field (Einternal) formed in the interface between p-type ZnCo2O4 and the n-type g-C3N4 semiconductor could speed up the electron transfer during the catalytic reaction. This thereby induces the high-efficiency PMS activation for rapid organic pollutant removal. As expected, the ZnCo2O4/g-C3N4 hybrid catalysts significantly outperformed individual ZnCo2O4 and g-C3N4 in catalytic oxidative degradation of norfloxacin (NOR) in the presence of PMS (95.3% removal of 20 mg L−1 of NOR in 120 min). Furthermore, the ZnCo2O4/g-C3N4-mediated PMS activation system was systematically studied in terms of the identification of reactive radicals, the impact of control factors, and the recyclability of the catalyst. The results of this study demonstrated the great potential of a built-in electric field-driven catalyst as a novel PMS activator for the remediation of contaminated water.

[1]  Hao Liu,et al.  Well-dispersed cobalt nanoparticles encapsulated on ZIF-8-derived N-doped porous carbon as an excellent peroxymonosulfate activator for sulfamethoxazole degradation , 2022, Chemical Engineering Journal.

[2]  Lifang Jiao,et al.  PEM water electrolysis for hydrogen production: fundamentals, advances, and prospects , 2022, Carbon Neutrality.

[3]  Yu-qiong Gao,et al.  Comparative investigation of diclofenac degradation by Fe2+/chlorine and Fe2+/PMS processes , 2022, Separation and Purification Technology.

[4]  Zhongyi Liu,et al.  Electrostatic self-assembly of 2D/2D CoWO4/g-C3N4 p—n heterojunction for improved photocatalytic hydrogen evolution: Built-in electric field modulated charge separation and mechanism unveiling , 2022, Nano Research.

[5]  Yue Sun,et al.  Assembly of UiO-66 onto Co-doped Fe3O4 nanoparticles to activate peroxymonosulfate for efficient degradation of fenitrothion and simultaneous in-situ adsorption of released phosphate. , 2022, Journal of hazardous materials.

[6]  Cui Ying Toe,et al.  Reconstructing Cu Nanoparticle Supported on Vertical Graphene Surfaces via Electrochemical Treatment to Tune the Selectivity of CO2 Reduction toward Valuable Products , 2022, ACS Catalysis.

[7]  Yu Qiu,et al.  Facile Synthesis of Highly Dispersed and Well-Alloyed Bimetallic Nanoparticles on Oxide Support. , 2022, Small.

[8]  T. Das,et al.  Advances on catalytic reduction of 4-nitrophenol by nanostructured materials as benchmark reaction , 2022, International Nano Letters.

[9]  T. Vo,et al.  Adsorption of norfloxacin from aqueous solution on biochar derived from spent coffee ground: Master variables and response surface method optimized adsorption process. , 2021, Chemosphere.

[10]  Yong Zhang,et al.  Z‐Scheme Flower‐Like SnO2/g‐C3N4 Composite with Sn2+ Active Center for Enhanced Visible‐Light Photocatalytic Activity , 2021, Advanced Sustainable Systems.

[11]  Z. Duan,et al.  Insights into active species of ultrafine iridium oxide nanoparticle electrocatalysts in hydrogen/oxygen evolution reactions , 2021 .

[12]  Jun Ma,et al.  Further understanding the role of hydroxylamine in transformation of reactive species in Fe(II)/peroxydisulfate system , 2021 .

[13]  Zhirong Sun,et al.  Preparation of metal organic framework derived materials CoFe2O4@NC and its application for degradation of norfloxacin from aqueous solutions by activated peroxymonosulfate. , 2021, Chemosphere.

[14]  Sabyasachi Ghosh,et al.  An environment friendly free-standing cellulose membrane derived for catalytic reduction of 4-nitrophenol: A sustainable approach , 2020 .

[15]  Haixia Wu,et al.  Degradation of norfloxacin with peroxymonosulfate activated by nanoconfinement Co3O4@CNT nanocomposite , 2020 .

[16]  Yongrong Yang,et al.  Boosting visible-light-driven hydrogen evolution from formic acid over AgPd/2D g-C3N4 nanosheets Mott-Schottky photocatalyst , 2020, Chemical Engineering Journal.

[17]  Kun Wu,et al.  Performance and mechanisms of sulfadiazine removal using persulfate activated by Fe3O4@CuOx hollow spheres. , 2020, Chemosphere.

[18]  Xin Lu,et al.  Novel magnetic biochar as an activator for peroxymonosulfate to degrade bisphenol A: Emphasizing the synergistic effect between graphitized structure and CoFe2O4 , 2020 .

[19]  P. Dutta,et al.  Nanoparticle processing: Understanding and controlling aggregation. , 2020, Advances in colloid and interface science.

[20]  Heng Liang,et al.  Sludge activated carbon-based CoFe2O4-SAC nanocomposites used as heterogeneous catalysts for degrading antibiotic norfloxacin through activating peroxymonosulfate , 2020, Chemical Engineering Journal.

[21]  Po-Chun Chen,et al.  P-type spinel ZnCo2O4 thin films prepared using sol-gel process , 2020 .

[22]  Zhaodong Nan,et al.  Highly efficient Fenton-like catalyst Fe-g-C3N4 porous nanosheets formation and catalytic mechanism , 2020 .

[23]  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.

[24]  Jianguo Jiang,et al.  Preparation, environmental application and prospect of biochar-supported metal nanoparticles: A review. , 2020, Journal of hazardous materials.

[25]  Yi-Feng Lin,et al.  Enhanced degradation of paracetamol in water using sulfate radical-based advanced oxidation processes catalyzed by 3-dimensional Co3O4 nanoflower , 2019, Chemical Engineering Journal.

[26]  F. Xiao,et al.  Porous Montmorillonite@Graphene Oxide@Au Nanoparticle Composite Microspheres for Organic Dye Degradation , 2019, ACS Applied Nano Materials.

[27]  B. Pan,et al.  Development of Fe-doped g-C3N4/graphite mediated peroxymonosulfate activation for degradation of aromatic pollutants via nonradical pathway. , 2019, The Science of the total environment.

[28]  W. Shi,et al.  Controllable synthesis of mesoporous manganese oxide microsphere efficient for photo-Fenton-like removal of fluoroquinolone antibiotics , 2019, Applied Catalysis B: Environmental.

[29]  Shengjiong Yang,et al.  Rational design and synthesis of hollow Co3O4@Fe2O3 core-shell nanostructure for the catalytic degradation of norfloxacin by coupling with peroxymonosulfate , 2019, Chemical Engineering Journal.

[30]  Peifang Wang,et al.  Oxygen vacancies and phosphorus codoped black titania coated carbon nanotube composite photocatalyst with efficient photocatalytic performance for the degradation of acetaminophen under visible light irradiation , 2018, Chemical Engineering Journal.

[31]  Yichun Liu,et al.  Immobilization of ultrafine Ag nanoparticles on well-designed hierarchically porous silica for high-performance catalysis. , 2018, Journal of colloid and interface science.

[32]  Juan Gao,et al.  Contribution of alcohol radicals to contaminant degradation in quenching studies of persulfate activation process. , 2018, Water research.

[33]  Hui Hu,et al.  Facile synthesis of ultrafine cobalt oxides embedded into N-doped carbon with superior activity in hydrogenation of 4-nitrophenol. , 2018, Journal of colloid and interface science.

[34]  B. Pan,et al.  Fe(III)-Doped g-C3N4 Mediated Peroxymonosulfate Activation for Selective Degradation of Phenolic Compounds via High-Valent Iron-Oxo Species. , 2018, Environmental science & technology.

[35]  Naiyun Gao,et al.  Activation of peroxymonosulfate by Al2O3-based CoFe2O4 for the degradation of sulfachloropyridazine sodium: Kinetics and mechanism , 2017 .

[36]  A. Moores,et al.  Novel Catalytic Materials for Energy and the Environment , 2017 .

[37]  H. Zeng,et al.  Photocatalysts fabricated by depositing plasmonic Ag nanoparticles on carbon quantum dots/graphitic carbon nitride for broad spectrum photocatalytic hydrogen generation , 2017 .

[38]  K. Nakanishi,et al.  Functionalization of hierarchically porous silica monoliths with polyethyleneimine (PEI) for CO2 adsorption , 2017 .

[39]  W. Ho,et al.  Hybridization of rutile TiO₂ (rTiO₂) with g-C₃N₄ quantum dots (CN QDs): An efficient visible-light-driven z-scheme hybridized photocatalyst , 2017 .

[40]  Teik-Thye Lim,et al.  Generation of sulfate radical through heterogeneous catalysis for organic contaminants removal: Current development, challenges and prospects , 2016 .

[41]  X. Niu,et al.  Retentions of bisphenol A and norfloxacin by three different ultrafiltration membranes in regard to drinking water treatment , 2016 .

[42]  Hui Cheng,et al.  ZnCo2O4 Quantum Dots Anchored on Nitrogen‐Doped Carbon Nanotubes as Reversible Oxygen Reduction/Evolution Electrocatalysts , 2016, Advanced materials.

[43]  Dong Yang,et al.  Synergistic Effect of Co3O4 Nanoparticles and Graphene as Catalysts for Peroxymonosulfate-Based Orange II Degradation with High Oxidant Utilization Efficiency , 2016 .

[44]  Limin Wang,et al.  Metal organic frameworks route to in situ insertion of multiwalled carbon nanotubes in Co3O4 polyhedra as anode materials for lithium-ion batteries. , 2015, ACS nano.

[45]  M. A. Woo,et al.  Electrochemical Synthesis of Spinel Type ZnCo2O4 Electrodes for Use as Oxygen Evolution Reaction Catalysts. , 2014, The journal of physical chemistry letters.

[46]  Jing Bai,et al.  Unusual Formation of ZnCo2O4 3D Hierarchical Twin Microspheres as a High‐Rate and Ultralong‐Life Lithium‐Ion Battery Anode Material , 2014 .

[47]  H. Ngo,et al.  A review on the occurrence of micropollutants in the aquatic environment and their fate and removal during wastewater treatment. , 2014, The Science of the total environment.

[48]  M. V. van Loosdrecht,et al.  Performance of aerobic granular sludge in a sequencing batch bioreactor exposed to ofloxacin, norfloxacin and ciprofloxacin. , 2014, Water research.

[49]  Abdullah M. Asiri,et al.  Ultrathin graphitic carbon nitride nanosheets: a low-cost, green, and highly efficient electrocatalyst toward the reduction of hydrogen peroxide and its glucose biosensing application. , 2013, Nanoscale.

[50]  Abdullah M. Asiri,et al.  Au-nanoparticle-loaded graphitic carbon nitride nanosheets: green photocatalytic synthesis and application toward the degradation of organic pollutants. , 2013, ACS applied materials & interfaces.

[51]  Wenju Jiang,et al.  Spectroscopic study of degradation products of ciprofloxacin, norfloxacin and lomefloxacin formed in ozonated wastewater. , 2012, Water research.

[52]  George P. Anipsitakis,et al.  Radical generation by the interaction of transition metals with common oxidants. , 2004, Environmental science & technology.

[53]  Qiang Xu,et al.  Metal–Organic Framework Templated Porous Carbon‐Metal Oxide/Reduced Graphene Oxide as Superior Support of Bimetallic Nanoparticles for Efficient Hydrogen Generation from Formic Acid , 2018 .