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gCN-P: a coupled g-C3N4/persulfate system for photocatalytic degradation of organic pollutants under simulated sunlight

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Abstract

A coupled g-C3N4/PDS system, named gCN-P, has been put forward to degrade refractory organic pollutants under simulated sunlight which integrates photocatalysis and PS-AOPs (advanced oxidation of persulfate based on sulfate radicals). The coupled g-C3N4 and PDS showed superior synergistic effect for MO degradation under simulated sunlight. Results showed that almost all MO was removed in the gCN-P system after irradiation for 80 min under simulated sunlight. The degradation rate of gCN-P system was improved by 12.6 and 4.9 times compared to single PDS and g-C3N4 systems, respectively. And only by adding 0.01 g of persulfate into the gCN-P system. The results of quenching experiments and EPR showed that O2−, 1O2 and h+ were main active species for the degradation of MO in the gCN-P system under simulated sunlight. Application of the gCN-P system in tap water samples demonstrated its excellent performance in real-world water environment, and the gCN-P system was employed for removing other new contaminants such as bisphenol A, ciprofloxacin, and paracetamol. The results demonstrated the gCN-P system can effectively remove organic pollutants under sunlight in practices.

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Data availability

The datasets used and/or analyzed during the current study are available from the corresponding author on reasonable request.

References

  • Azari A, Nabizadeh R, Nasseri S, Mahvi AH, Mesdaghinia AR (2020) Comprehensive systematic review and meta-analysis of dyes adsorption by carbon-based adsorbent materials: classification and analysis of last decade studies. Chemosphere 250:126238

    Article  CAS  Google Scholar 

  • Chen J, Ollis DF, Rulkens WH, Bruning H (1999) Kinetic processes of photocatalytic mineralization of alcohols on metallized titanium dioxide. Water Res 33:1173–1180

    Article  CAS  Google Scholar 

  • Dewil R, Mantzavinos D, Poulios I, Rodrigo MA (2017) New perspectives for advanced oxidation processes. J Environ Manage 195:93–99

    Article  CAS  Google Scholar 

  • Das KK, Patnaik S, Mansingh S, Behera A, Mohanty A, Acharya C, Parida KM (2020) Enhanced photocatalytic activities of polypyrrole sensitized zinc ferrite/graphitic carbon nitride n-n heterojunction towards ciprofloxacin degradation, hydrogen evolution and antibacterial studies. J Colloid Interface Sci 561:551–567

    Article  CAS  Google Scholar 

  • Dhanalakshmi KB, Anandan S, Madhavan J, Maruthamuthu P (2008) Photocatalytic degradation of phenol over TiO2 powder: the influence of peroxomonosulphate and peroxodisulphate on the reaction rate. Sol Energy Mater Sol Cells 92:457–463

    Article  CAS  Google Scholar 

  • Dong F, Wu LW, Sun YJ, Fu M, Wu ZB, Lee SC (2011) Efficient synthesis of polymeric g-C3N4 layered materials as novel efficient visible light driven photocatalysts. J Mater Chem 21:15171–15174

    Article  CAS  Google Scholar 

  • Du X, Bai X, Xu L, Yang L, Jin P (2020) Visible-light activation of persulfate by TiO2/g-C3N4 photocatalyst toward efficient degradation of micropollutants. Chem Eng J 384:123245

    Article  CAS  Google Scholar 

  • Edilson do Vale-Júnior, SD, Irene Garcia Cano, Josep Maria Guilemany, Sergi Garcia-Segura, Carlos Alberto Martínez-Huitle (2016) Acid blue 29 decolorization and mineralization by anodic oxidation with a cold gas spray synthesized SneCueSb alloy anode. Chemosphere 148: 47-54

  • Fernandes A, Makos P, Wang Z, Boczkaj G (2020) Synergistic effect of TiO2 photocatalytic advanced oxidation processes in the treatment of refinery effluents. Chem Eng J 391:123488

    Article  CAS  Google Scholar 

  • Feng CY, Diao P (2021) Nickel foam supported NiFe2O4-NiO hybrid: a novel 3D porous catalyst for efficient heterogeneous catalytic ozonation of azo dye and nitrobenzene. Appl Surf Sci 541:148683

    Article  CAS  Google Scholar 

  • Furman OS, Teel AL, Watts RJ (2010) Mechanism of base activation of persulfate. Environ Sci Technol 44:6423–6428

    Article  CAS  Google Scholar 

  • Ghanbari F, Moradi M (2017) Application of peroxymonosulfate and its activation methods for degradation of environmental organic pollutants: Review. Chem Eng J 310:41–62

    Article  CAS  Google Scholar 

  • Gągol M, Przyjazny A, Boczkaj G (2018) Effective method of treatment of industrial effluents under basic pH conditions using acoustic cavitation-a comprehensive comparison with hydrodynamic cavitation processes. Chemical Engineering and Processing-Process Intensification 128:103–113

    Article  Google Scholar 

  • Hasija V, Nguyen VH, Kumar A, Raizada P, Krishnan V, Khan AAP, Singh P, Lichtfouse E, Wang C, Thi Huong P (2021) Advanced activation of persulfate by polymeric g-C3N4 based photocatalysts for environmental remediation: A review. J Hazard Mater 413:125324

    Article  CAS  Google Scholar 

  • Ike IA, Linden KG, Orbell JD, Duke M (2018) Critical review of the science and sustainability of persulphate advanced oxidation processes. Chem Eng J 338:651–669

    Article  CAS  Google Scholar 

  • Jiang JJ, Wang XY, Zhang CJ, Li TR, Lin YH, Xie TF, Dong SS (2020) Porous 0D/3D NiCo2O4/g-C3N4 accelerate emerging pollutant degradation in PMS/vis system: degradation mechanism, pathway and toxicity assessment. Chem Eng J 397:125356

    Article  CAS  Google Scholar 

  • Jagannathan M, Grieser F, Ashokkumar M (2013) Sonophotocatalytic degradation of paracetamol using TiO2 and Fe3+. Sep Purif Technol 103:114–118

    Article  CAS  Google Scholar 

  • Jawad A, Zhan K, Wang HB, Shahzad A, Zeng ZH, Wang J, Zhou XQ, Ullah H, Chen ZL, Chen ZQ (2020) Tuning of persulfate activation from a free radical to a nonradical pathway through the incorporation of non-redox magnesium oxide. Environ Sci Technol 54:2476–2488

    Article  CAS  Google Scholar 

  • Jiang XW, Li J, Fang J, Gao L, Cai WX, Li XX, Xu AH, Ruan XC (2017) The photocatalytic performance of g-C3N4 from melamine hydrochloride for dyes degradation with peroxymonosulfate. J Photochem Photobiol A Chem 336:54–62

    Article  CAS  Google Scholar 

  • Kong L, Fang G, Xi X, Wen Y, Chen Y, Xie M, Zhu F, Zhou D, Zhan J (2021) A novel peroxymonosulfate activation process by periclase for efficient singlet oxygen-mediated degradation of organic pollutants. Chem Eng J 403:126445

    Article  CAS  Google Scholar 

  • Kumar A, Raizada P, Singh P, Saini RV, Saini AK, Hosseini-Bandegharaei A (2020) Perspective and status of polymeric graphitic carbon nitride based Z-scheme photocatalytic systems for sustainable photocatalytic water purification. Chem Eng J 391:123496

    Article  CAS  Google Scholar 

  • Li HP, Wang Z, Lu YX, Liu S, Chen XJ, Wei GY, Ye G, Chen J (2020) Microplasma electrochemistry (MIPEC) methods for improving the photocatalytic performance of g-C3N4 in degradation of RhB. Appl Surf Sci 531:147307

    Article  CAS  Google Scholar 

  • Liang QQ, Yu LH, Jiang W, Zhou S, Zhong ST, Jiang W (2017) One-pot synthesis of magnetic graphitic carbon nitride photocatalyst with synergistic catalytic performance under visible-light irradiation. J Photochem Photobiol A Chem 335:165–173

    Article  CAS  Google Scholar 

  • Liu B, Qiao M, Wang Y, Wang L, Gong Y, Guo T, Zhao X (2017) Persulfate enhanced photocatalytic degradation of bisphenol A by g-C3N4 nanosheets under visible light irradiation. Chemosphere 189:115–122

    Article  CAS  Google Scholar 

  • Liu CY, Huang HW, Du X, Zhang TR, Tian N, Guo YX, Zhang YH (2015) In situ co-crystallization for fabrication of g-c3n4/bi5o7i heterojunction for enhanced visible-light photocatalysis. J Phys Chem C 119:17156–17165

    Article  CAS  Google Scholar 

  • Lominchar MA, Santos A, de Miguel E, Romero A (2018) Remediation of aged diesel contaminated soil by alkaline activated persulfate. Sci Total Environ 622–623:41–48

    Article  Google Scholar 

  • Lutze HV, Kerlin N, Schmidt TC (2015) Sulfate radical-based water treatment in presence of chloride: formation of chlorate, inter-conversion of sulfate radicals into hydroxyl radicals and influence of bicarbonate. Water Res 72:349–360

    Article  CAS  Google Scholar 

  • Madhavan J, Muthuraaman B, Murugesan S, Anandan S, Maruthamuthu P (2006) Peroxoraonosulphate, an efficient oxidant for the photocatalysed degradation of a textile dye, acid red 88. Sol Energy Mater Sol Cells 90:1875–1887

    Article  CAS  Google Scholar 

  • Melian EP, Diaz OG, Rodriguez JMD, Arana J, Pena JP (2013) Adsorption and photocatalytic degradation of 2,4-dichlorophenol in TiO2 suspensions. Effect of hydrogen peroxide, sodium peroxodisulphate and ozone. Appl Catal A Gen 455:227–233

    Article  CAS  Google Scholar 

  • Mousavi M, Habibi-Yangjeh A, Abitorabi M (2016) Fabrication of novel magnetically separable nanocomposites using graphitic carbon nitride, silver phosphate and silver chloride and their applications in photocatalytic removal of different pollutants using visible-light irradiation. J Colloid Interface Sci 480:218–231

    Article  CAS  Google Scholar 

  • Neppolian B, Celik E, Choi H (2008) Photochemical oxidation of arsenic(III) to arsenic(V) using peroxydisulfate ions as an oxidizing agent. Environ Sci Technol 42:6179–6184

    Article  CAS  Google Scholar 

  • Ong WJ, Tan LL, Ng YH, Yong ST, Chai SP (2016) Graphitic carbon nitride (g-C3N4)-based photocatalysts for artificial photosynthesis and environmental remediation: are we a step closer to achieving sustainability? Chem Rev 116:7159–7329

    Article  CAS  Google Scholar 

  • Orooji Y, Ghanbari M, Amiri O, Salavati-Niasari M (2020) Facile fabrication of silver iodide/graphitic carbon nitride nanocomposites by notable photo-catalytic performance through sunlight and antimicrobial activity. J Hazard Mater 389:122079

    Article  CAS  Google Scholar 

  • Qian HY, Huang HJ, Wang X (2015) Design and synthesis of palladium/graphitic carbon nitride/carbon black hybrids as high-performance catalysts for formic acid and methanol electrooxidation. J Power Sources 275:734–741

    Article  CAS  Google Scholar 

  • Reddy CV, Reddy KR, Harish VVN, Shim J, Shankar MV, Shetti NP, Aminabhavi TM (2020) Metal-organic frameworks (MOFs)-based efficient heterogeneous photocatalysts: Synthesis, properties and its applications in photocatalytic hydrogen generation, CO2 reduction and photodegradation of organic dyes. ScienceDirect 45:7656–7679

    CAS  Google Scholar 

  • Rong XS, Qiu FX, Zhao H, Yan J, Zhu XL, Yang DY (2015) Fabrication of Single-layer graphitic carbon nitride and coupled systems for the photocatalytic degradation of dyes under visible-light irradiation. Eur J Inorg Chem 8:1359–1367

    Article  Google Scholar 

  • Sharma VK, Feng MB (2019) Water depollution using metal-organic frameworks-catalyzed advanced oxidation processes: A review. J Hazard Mater 372:3–16

    Article  CAS  Google Scholar 

  • Shang Y, Chen C, Zhang P, Yue Q, Li Y, Gao B, Xu X (2019) Removal of sulfamethoxazole from water via activation of persulfate by Fe3C@NCNTs including mechanism of radical and nonradical process. Chem Eng J 375:122004

    Article  CAS  Google Scholar 

  • Song Y, Huang L, Zhang X, Zhang H, Wang L, Zhang H, Liu Y (2020) Synergistic effect of persulfate and g-C3N4 under simulated solar light irradiation: implication for the degradation of sulfamethoxazole. J Hazard Mater 393:122379

    Article  CAS  Google Scholar 

  • Song YL, Shao PH, Tian JY, Shi WX, Gao SS, Qi JY, Yan XJ, Cui FY (2016) One-step hydrothermal synthesis of ZnO hollow nanospheres uniformly grown on graphene for enhanced photocatalytic performance. Ceram Int 42:2074–2078

    Article  CAS  Google Scholar 

  • Tang SF, Wang ZT, Yuan DL, Zhang C, Rao YD, Wang ZB, Yin K (2020) Ferrous ion-tartaric acid chelation promoted calcium peroxide fenton-like reactions for simulated organic wastewater treatment. Journal Clean Prod 268:122253

    Article  CAS  Google Scholar 

  • Tang M, Ao Y, Wang C, Wang P (2020) Facile synthesis of dual Z-scheme g-C3N4/Ag3PO4/AgI composite photocatalysts with enhanced performance for the degradation of a typical neonicotinoid pesticide. Appl Catal B Environ 268:118395

    Article  CAS  Google Scholar 

  • Tao YF, Ni Q, Wei MY, Xia DS, Li XX, Xu AH (2015) Metal-free activation of peroxymonosulfate by g-C3N4 under visible light irradiation for the degradation of organic dyes. Rsc Adv 5(55):44128–44136

    Article  CAS  Google Scholar 

  • Thomas A, Fischer A, Goettmann F, Antonietti M, Muller JO, Schlogl R, Carlsson JM (2008) Graphitic carbon nitride materials: variation of structure and morphology and their use as metal-free catalysts. J Mater Chem 18(41):4893–4908

    Article  CAS  Google Scholar 

  • Tong H, Ouyang SX, Bi YP, Umezawa N, Oshikiri M, Ye JH (2012) Nano-photocatalytic materials: possibilities and challenges. Adv Mater 24(2):229–251

    Article  CAS  Google Scholar 

  • Tsitonaki A, Petri B, Crimi M, MosbaeK H, Siegrist RL, Bjerg PL (2010) In situ chemical oxidation of contaminated soil and groundwater using persulfate: a review. Crit Rev Env Sci Technol 40(1):55–91

    Article  CAS  Google Scholar 

  • Wang Y, Rao L, Wang P, Shi Z, Zhang L (2020) Photocatalytic activity of N-TiO2/O-doped N vacancy g-C3N4 and the intermediates toxicity evaluation under tetracycline hydrochloride and Cr (VI) coexistence environment. Appl Catal B Environ 262:118308

    Article  CAS  Google Scholar 

  • Wang YB, Zhao X, Cao D, Wang Y, Zhu YF (2017a) Peroxymonosulfate enhanced visible light photocatalytic degradation bisphenol A by single-atom dispersed Ag mesoporous g-C3N4 hybrid. Appl Catal B Environ 211:79–88

    Article  CAS  Google Scholar 

  • Wang YB, Cao D, Zhao X (2017b) Heterogeneous degradation of refractory pollutants by peroxymonosulfate activated by CoOx-doped ordered mesoporous carbon. Chem Eng J 328:1112–1121

    Article  CAS  Google Scholar 

  • Xie P, Ma J, Liu W, Zou J, Yue S, Li X, Wiesner MR, Fang J (2015) Removal of 2-MIB and geosmin using UV/persulfate: contributions of hydroxyl and sulfate radicals. Water Res 69:223–233

    Article  CAS  Google Scholar 

  • Xu CY, Han Q, Zhao Y, Wang LX, Li Y, Qu LT (2015) Sulfur-doped graphitic carbon nitride decorated with graphene quantum dots for an efficient metal-free electrocatalyst. J Mater Chem A 3(5):1841–1846

    Article  CAS  Google Scholar 

  • Yang B, Mao XH, Pi L, Wu YX, Ding HJ, Zhang WH (2017) Effect of pH on the adsorption and photocatalytic degradation of sulfadimidine in Vis/g-C3N4 progress. Environ Sci Pollut Res 24(9):8658–8670

    Article  CAS  Google Scholar 

  • Ye YC, Yang H, Zhang HM, Jiang JL (2020) A promising Ag2CrO4/LaFeO3 heterojunction photocatalyst applied to photo-Fenton degradation of RhB. Environ Technol 41(12):1486–1503

    Article  CAS  Google Scholar 

  • Yin Z, Han MG, Hu Z, Feng L, Liu YZ, Du ZW, Zhang LQ (2020) Peroxymonosulfate enhancing visible light photocatalytic degradation of bezafibrate by Pd/g-C3N4 catalysts: The role of sulfate radicals and hydroxyl radicals. Chem Eng J 390:124532

    Article  CAS  Google Scholar 

  • Zhang JJ, Zhao X, Wang YB, Gong Y, Cao D, Qiao M (2018) Peroxymonosulfate-enhanced visible light photocatalytic degradation of bisphenol A by perylene imide-modified g-C3N4. Appl Catal B Environ 237:976–985

    Article  CAS  Google Scholar 

  • Zhu B, Xia PF, Ho WK, Yu JG (2015) Isoelectric point and adsorption activity of porous g-C3N4. Appl Surf Sci 344:188–195

    Article  CAS  Google Scholar 

  • Zhu SS, Huang XC, Ma F, Wang L, Duan XG, Wang SB (2018) Catalytic removal of aqueous contaminants on N-doped graphitic biochars: inherent roles of adsorption and nonradical mechanisms. Environ Sci Technol 52(15):8649–8658

    Article  CAS  Google Scholar 

  • Zhu WY, Sun FQ, Goei R, Zhou Y (2017) Facile fabrication of RGO-WO3 composites for effective visible light photocatalytic degradation of sulfamethoxazole. Appl Catal B Environ 207:93–102

    Article  CAS  Google Scholar 

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Funding

This study was supported by the National Natural Science Foundation of China (No. 51779132).

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  1. School of Environmental Science and Engineering, Shandong University, Qingdao, 266237, People’s Republic of China

    Mengdi Shen, Xiaodong Zhang, Shan Zhao & Shuguang Wang

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  1. Mengdi Shen
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  2. Xiaodong Zhang
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  3. Shan Zhao
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Contributions

Mengdi Shen: conceptualization, methodology, validation, investigation, writing—original draft, data curation, formal analysis, writing—review and editing. Xiaodong Zhang: conceptualization, supervision, writing—review and editing, resources, funding acquisition, data curation. Shan Zhao: conceptualization, supervision, resources. Shuguang Wang: supervision, conceptualization.

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Correspondence to Xiaodong Zhang.

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Shen, M., Zhang, X., Zhao, S. et al. gCN-P: a coupled g-C3N4/persulfate system for photocatalytic degradation of organic pollutants under simulated sunlight. Environ Sci Pollut Res 29, 23280–23291 (2022). https://doi.org/10.1007/s11356-021-17540-0

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