Photocatalysis-self-Fenton system over edge covalently modified g-C3N4 with high mineralization of persistent organic pollutants.

The Fenton process is a widely used to remedy organic wastewaters, but it has problems of adding H2O2, low utilization efficiency of H2O2 and low mineralization efficiency. Here, a new photocatalysis-self-Fenton process was exploited for the removal of persistent 4-chlorophenol (4-CP) pollutant through coupling the photocatalysis of 4-carboxyphenylboronic acid edge covalently modified g-C3N4 (CPBA-CN) with Fenton. In this process, H2O2 was in situ generated via photocatalysis over CPBA-CN, the photogenerated electrons assisted the accelerated regeneration of Fe2+ to improve the utilization efficiency of H2O2, and the photogenerated holes facilitated the enhancement of 4-CP mineralization. Under the conjugation of CPBA, the electronic structure of CN was optimized and the molecular dipole was enhanced, resulting in the deepening valence band position, accelerated electron-hole pair separation, and improved O2 adsorption-activation. Therefore, the incremental 4-CP degradation rate in the CPBA-CN photocatalysis-self-Fenton process was approaching 0.099 min-1, by a factor of 3.1 times compared with photocatalysis. The parallel mineralization efficiency increased to 74.6% that was 2.1 and 2.6 times than photocatalysis and Fenton, respectively. In addition, this system maintained an excellent stability in the recycle experiment and can be potentially applied in a wide range of pHs and under the coexistence of various ions. This study would provide new insights for improving Fenton process and promote further development of Fenton in organic wastewater purification.

[1]  F. Feng,et al.  Activating C–H Bonds by Tuning Fe Sites and an Interfacial Effect for Enhanced Methanol Oxidation , 2022, Advanced materials.

[2]  İ. Şentürk,et al.  Degradation of phenol and 4-chlorophenol from aqueous solution by Fenton, photo-Fenton, sono-Fenton, and sono-photo-Fenton methods , 2022, Journal of the Iranian Chemical Society.

[3]  Jiaguo Yu,et al.  Calcination-regulated Microstructures of Donor-Acceptor Polymers towards Enhanced and Stable Photocatalytic H2O2 Production in Pure Water. , 2022, Angewandte Chemie.

[4]  Huixiang Wu,et al.  Strategies and challenges on selective electrochemical hydrogen peroxide production: Catalyst and reaction medium design , 2022, Chem Catalysis.

[5]  Yingping Huang,et al.  Functional Carbon Nitride Materials in Photo‐Fenton‐Like Catalysis for Environmental Remediation , 2022, Advanced Functional Materials.

[6]  Yong Zhu,et al.  Resin-based photo-self-Fenton system with intensive mineralization by the synergistic effect of holes and hydroxyl radicals , 2022, Applied Catalysis B: Environmental.

[7]  Jiaguo Yu,et al.  Promoting intramolecular charge transfer of graphitic carbon nitride by donor–acceptor modulation for visible‐light photocatalytic H2 evolution , 2022, Interdisciplinary Materials.

[8]  Zhouping Wang,et al.  Unprecedentedly efficient mineralization performance of photocatalysis-self-Fenton system towards organic pollutants over oxygen-doped porous g-C3N4 nanosheets , 2022, Applied Catalysis B: Environmental.

[9]  Changyong Zhang,et al.  Hydroxyl radicals in anodic oxidation systems: generation, identification and quantification. , 2022, Water research.

[10]  Yang Liao,et al.  Significantly improved photocatalysis-self-Fenton degradation performance over g-C3N4 via promoting Fe(III)/Fe(II) cycle , 2022, Rare Metals.

[11]  M. K. Rofouei,et al.  A novel Z-scheme oxygen-doped g-C3N4 nanosheet/NaBiS2 nanoribbon for efficient photocatalytic H2O2 production and organic pollutants degradation , 2022, Journal of Physics and Chemistry of Solids.

[12]  Xinru Liu,et al.  Photocatalytic H2O2 production driven by cyclodextrin-pyrimidine polymer in a wide pH range without electron donor or oxygen aeration , 2022, Applied Catalysis B: Environmental.

[13]  Nan Li,et al.  Activated Ni-based metal-organic framework catalyst with well-defined structure for electrosynthesis of hydrogen peroxide , 2022, Chemical Engineering Journal.

[14]  Yong Zhou,et al.  Boosting O2 Reduction and H2O Dehydrogenation Kinetics: Surface N‐Hydroxymethylation of g‐C3N4 Photocatalysts for the Efficient Production of H2O2 , 2021, Advanced Functional Materials.

[15]  D. Çifçi,et al.  Comparison of kinetics and costs of Fenton and photo-Fenton processes used for the treatment of a textile industry wastewater. , 2021, Journal of environmental management.

[16]  Jiahai Ma,et al.  Concerted high innergenerated-H2O2 photocatalysis and Photo-Fenton degradation of organic pollutants over SCNO@CdS , 2021 .

[17]  Yumeng Wang,et al.  Enhanced Fenton-like process via interfacial electron donating of pollutants over in situ Cobalt-doped graphitic carbon nitride. , 2021, Journal of colloid and interface science.

[18]  Peifang Wang,et al.  Iodide-Induced Fragmentation of Polymerized Hydrophilic Carbon Nitride for High Performance Quasi-Homogeneous Photocatalytic H2O2 Production. , 2021, Angewandte Chemie.

[19]  Changling Yu,et al.  Photocatalytic H2O2 production and removal of Cr (VI) via a novel Lu3NbO7: Yb, Ho/CQDs/AgInS2/In2S3 heterostructure with broad spectral response. , 2021, Journal of hazardous materials.

[20]  Hui Huang,et al.  In-situ photovoltage transients assisted catalytic study on H2O2 photoproduction over organic molecules modified carbon nitride photocatalyst , 2021 .

[21]  Yanmei Zheng,et al.  Rapid Microwave Synthesis of Mesoporous Oxygen-Doped g-C3N4 with Carbon Vacancies for Efficient Photocatalytic H2O2 Production , 2021 .

[22]  Xinchen Wang,et al.  Biomimetic Donor-Acceptor Motifs in Carbon Nitrides: Enhancing Red-Light Photocatalytic Selective Oxidation by Rational Surface Engineering , 2021 .

[23]  Xiwang Zhang,et al.  Photoredox catalysis over semiconductors for light-driven hydrogen peroxide production , 2021 .

[24]  Yupeng Yuan,et al.  Unravelling intramolecular charge transfer in donor–acceptor structured g-C3N4 for superior photocatalytic hydrogen evolution , 2021, Journal of Materials Chemistry A.

[25]  L. Qu,et al.  Functional group defect design in polymeric carbon nitride for photocatalytic application , 2020 .

[26]  W. Yao,et al.  Photocatalysis-self-Fenton system with high-fluent degradation and high mineralization ability , 2020 .

[27]  C. Su,et al.  Intrinsic Defects in Polymetric Carbon Nitride for Photocatalysis Applications. , 2020, Chemistry, an Asian journal.

[28]  Xiwang Zhang,et al.  Carbon-based materials for photo- and electrocatalytic synthesis of hydrogen peroxide. , 2020, Nanoscale.

[29]  Shen-ming Chen,et al.  MoN Nanorod/Sulfur-Doped Graphitic Carbon Nitride for Electrochemical Determination of Chloramphenicol , 2020 .

[30]  Huijuan Liu,et al.  Carbon nanodot-modified FeOCl for photo-assisted Fenton reaction featuring synergistic in-situ H2O2 production and activation , 2020 .

[31]  J. Xiong,et al.  CN/rGO@BPQDs high-low junctions with stretching spatial charge separation ability for photocatalytic degradation and H2O2 production , 2020 .

[32]  K. Domen,et al.  Spatially separating redox centers on 2D carbon nitride with cobalt single atom for photocatalytic H2O2 production , 2020, Proceedings of the National Academy of Sciences.

[33]  V. Yargeau,et al.  Oxidation of tetracycline and oxytetracycline for the photo-Fenton process: Their transformation products and toxicity assessment. , 2020, Water research.

[34]  N. Tang,et al.  Increasing Solar Absorption of Atomically Thin 2D Carbon Nitride Sheets for Enhanced Visible‐Light Photocatalysis , 2019, Advanced materials.

[35]  Lirong Zheng,et al.  Solar Irradiation Induced Transformation of Ferrihydrite in the Presence of Aqueous Fe2. , 2019, Environmental science & technology.

[36]  Liang Zhao,et al.  A review on Fenton process for organic wastewater treatment based on optimization perspective. , 2019, The Science of the total environment.

[37]  M. M. Bello,et al.  A review on approaches for addressing the limitations of Fenton oxidation for recalcitrant wastewater treatment , 2018, Process Safety and Environmental Protection.

[38]  Huilin Hou,et al.  Production of hydrogen peroxide through photocatalytic processes: a critical review of recent advances. , 2020, Angewandte Chemie.

[39]  Fengbao Zhang,et al.  Hierarchical photocatalyst of In2S3 on exfoliated MoS2 nanosheets for enhanced visible-light-driven Aza-Henry reaction , 2018, Applied Catalysis B: Environmental.

[40]  Shu Hu,et al.  Photocatalytic hydrogen peroxide production by anthraquinone-augmented polymeric carbon nitride , 2018, Applied Catalysis B: Environmental.

[41]  Bo Yang,et al.  Carbon nanotubes covalent combined with graphitic carbon nitride for photocatalytic hydrogen peroxide production under visible light , 2018 .

[42]  Qing Wang,et al.  Industrial water pollution, water environment treatment, and health risks in China. , 2016, Environmental pollution.

[43]  Xizhang Wang,et al.  Can boron and nitrogen co-doping improve oxygen reduction reaction activity of carbon nanotubes? , 2013, Journal of the American Chemical Society.

[44]  Bifunctional Carbon Nitride Exhibiting both Enhanced Photoactivity and Residual Catalytic Activity in the Post-Irradiation Dark Period , 2022 .

[45]  Xingzhong Yuan,et al.  Defective polymeric carbon nitride: Fabrications, photocatalytic applications and perspectives , 2022 .