Skip to main content
Log in

Role of precursors on the photophysical properties of carbon nitride and its application for antibiotic degradation

  • Research Article
  • Published:
Environmental Science and Pollution Research Aims and scope Submit manuscript

Abstract

In this paper, we provide a comprehensive evaluation of graphitic carbon nitride (C3N4) powders derived from the four different precursors melamine, cyanamide, thiourea, and urea for the photocatalytic degradation of tetracycline (TC) antibiotic under sunlight irradiation. The powders were synthesized by employing the conventional thermal decomposition method. The synthesized powders were examined using different characterization tools for evaluating the photophysical properties. The degradation profile revealed that urea-derived C3N4 showed the highest activity while melamine-derived C3N4 showed the least activity. The TC degradation efficiency of the photocatalyst was found to be influenced more by the surface area values despite extended absorption by melamine in the visible light region. Stability tests on urea-derived C3N4 and others were checked by four runs of TC degradation under sunlight irradiation. The synthesized C3N4 powders also confirmed the dominance of urea-derived powders for cyclic stability.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8
Fig. 9
Fig. 10
Fig. 11
Fig. 12
Fig. 13
Fig. 14

Similar content being viewed by others

References

  • Addamo M, Augugliaro V, Paola AD, GarcĂ­a-LĂłpez E, Loddo V, Marcì G, Palmisano L (2005) Removal of drugs in aqueous systems by photoassisted degradation. J Appl Elecrtrochem 35:765–774

  • Ai C, Zhou D, Wang Q, Shao X, Lei Y (2015) Optimization of operating parameters for photocatalytic degradation of tetracycline using In2S3 under natural solar radiation. Sol Energy 113:34–42

    Article  CAS  Google Scholar 

  • Angleraud B, Mubumbila N, Tessier PY, Fernandez V, Turban G (2001) Bonding structure of carbon nitride films deposited by reactive plasma beam sputtering. Diam Relat Mater 10:1142–1146

    Article  CAS  Google Scholar 

  • Banerjee S, Pillai SC, Falaras P, O’Shea KE, Byrne JA, Dionysiou DD (2014) New insights into the mechanism of visible light photocatalysis. J Phys Chem Lett 5:2543–2554

    Article  CAS  Google Scholar 

  • Bu D, Zhuang H (2013) Biotemplated synthesis of high specific surface area copper-doped hollow spherical titania and its photocatalytic research for degradating chlorotetracycline. Appl Surf Sci 265:677–685

    Article  CAS  Google Scholar 

  • Cao S, Low J, Yu J, Jaroniec M (2015) Polymeric photocatalysts based on graphitic carbon nitride. Adv Mater 27:2150–2176

    Article  CAS  Google Scholar 

  • Dong F, Zhao Z, Xiong T, Ni Z, Zhang W, Sun Y, Ho W-K (2013) In situ construction of g-C3N4/g-C3N4 metal-free heterojunction for enhanced visible-light photocatalysis. ACS Appl Mater Interfaces 5:11392–11401

    Article  CAS  Google Scholar 

  • Fagan R, McCormack D, Hinder S, Pillai S (2016) Photocatalytic properties of g-C3N4–TiO2 heterojunctions under UV and visible light conditions. Materials 9:286

    Article  Google Scholar 

  • Fan X, Xing Z, Shu Z, Zhang L, Wang L, Shi J (2015) Improved photocatalytic activity of g-C3N4 derived from cyanamide-urea solution. RSC Adv 5:8323–8328

    Article  CAS  Google Scholar 

  • Fang J, Fan H, Li M, Long C (2015) Nitrogen self-doped graphitic carbon nitride as efficient visible light photocatalyst for hydrogen evolution. J Mater Chem A 3:13819–13826

    Article  CAS  Google Scholar 

  • Hao R, Wang G, Tang H, Sun L, Xu C, Han D (2016) Template-free preparation of macro/mesoporous g-C3N4/TiO2 heterojunction photocatalysts with enhanced visible light photocatalytic activity. Appl. Catal. B 187:47–58

    Article  CAS  Google Scholar 

  • He Y, Cai J, Zhang L, Wang X, Lin H, Teng B, Zhao L, Weng W, Wan H, Fan M (2014) Comparing two new composite photocatalysts, t-LaVO4/g-C3N4 and m-LaVO4/g-C3N4, for their structures and performances. Ind Eng Chem Res 53:5905–5915

    Article  CAS  Google Scholar 

  • Jeong J, Song W, Cooper WJ, Jung J, Greaves J (2010) Degradation of tetracycline antibiotics: mechanisms and kinetic studies for advanced oxidation/reduction processes. Chemosphere 78:533–540

    Article  CAS  Google Scholar 

  • Joy M, Nair BN, Mohamed AAP, Warrier KG, Hareesh UNS (2016) One-pot hydrothermal synthesis of visible-light-responsive MoS2/g-CNO heterostructures for organic-pollutant degradation. Eur. J. Inorg. Chem. 3912–3920

  • Kroke E (2014) Gt-C3N4—the first stable binary carbon(IV) nitride. Angew Chem Int Ed 53:11134–11136

    Article  CAS  Google Scholar 

  • Li J, Zhou M, Ye Z, Wang H, Ma C, Huo P, Yan Y (2015) Enhanced photocatalytic activity of g-C3N4-ZnO/HNT composite heterostructure photocatalysts for degradation of tetracycline under visible light irradiation. RSC Adv 5:91177–91189

    Article  CAS  Google Scholar 

  • Liu G, Niu P, Sun C, Smith SC, Chen Z, Lu GQ, Cheng H-M (2010) Unique electronic structure induced high photoreactivity of sulfur-doped graphitic C3N4. J Am Chem Soc 132:11642–11648

    Article  CAS  Google Scholar 

  • Liu J, Wang H, Antonietti M (2016) Graphitic carbon nitride “reloaded”: emerging applications beyond (photo)catalysis. Chem Soc Rev 45:2308–2326

    Article  CAS  Google Scholar 

  • Lotsch BV, Döblinger M, Sehnert J, Seyfarth L, Senker J, Oeckler O, Schnick W (2007) Unmasking melon by a complementary approach employing electron diffraction, solid-state NMR spectroscopy, and theoretical calculations—structural characterization of a carbon nitride polymer. Chem Eur J 13:4969–4980

    Article  CAS  Google Scholar 

  • LuĂ©vano-HipĂłlito E, MartĂ­nez-de la Cruz A, LĂłpez CuĂ©llar E (2016) Performance of ZnO synthesized by sol-gel as photocatalyst in the photooxidation reaction of NO. Environ. Sci. Pollut. Res 1–11

  • Luo B, Xu D, Li D, Wu G, Wu M, Shi W, Chen M (2015) Fabrication of a Ag/Bi3TaO7 plasmonic photocatalyst with enhanced photocatalytic activity for degradation of tetracycline. ACS Appl Mater Interfaces 7:17061–17069

    Article  CAS  Google Scholar 

  • Ma S, Zhan S, Jia Y, Shi Q, Zhou Q (2016) Enhanced disinfection application of Ag-modified g-C3N4 composite under visible light. Appl. Catal. B 186:77–87

    Article  CAS  Google Scholar 

  • Niu P, Liu G, Cheng H-M (2012) Nitrogen vacancy-promoted photocatalytic activity of graphitic carbon nitride. J Phys Chem C 116:11013–11018

    Article  CAS  Google Scholar 

  • Ong W-J, Tan L-L, Ng YH, Yong S-T, Chai S-P (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 

  • Panneri S, Ganguly P, Nair BN, Mohamed AAP, Warrier KG, Hareesh UNS (2016) Copyrolysed C3N4-Ag/ZnO ternary heterostructure systems for enhanced adsorption and photocatalytic degradation of tetracycline. Eur J Inorg Chem DOI. doi:10.1002/ejic.201600646

    Google Scholar 

  • Ren H-T, Jia S-Y, Wu Y, Wu S-H, Zhang T-H, Han X (2014) Improved photochemical reactivities of Ag2O/g-C3N4 in phenol degradation under UV and visible light. Ind Eng Chem Res 53:17645–17653

    Article  CAS  Google Scholar 

  • Reyes C, Fernández J, Freer J, Mondaca MA, Zaror C, Malato S, Mansilla HD (2006) Degradation and inactivation of tetracycline by TiO2 photocatalysis. J Photochem Photobiol A 184:141–146

    Article  CAS  Google Scholar 

  • Safari GH, Hoseini M, Seyedsalehi M, Kamani H, Jaafari J, Mahvi AH (2014) Photocatalytic degradation of tetracycline using nanosized titanium dioxide in aqueous solution. Int J Environ Sci Technol 12:603–616

    Article  Google Scholar 

  • Smitha VS, Jyothi CK, Mohamed AP, Pillai S, Warrier KG (2013) Novel multifunctional titania-silica-lanthanum phosphate nanocomposite coatings through an all aqueous sol-gel process. Dalton Trans 42:4602–4612

    Article  CAS  Google Scholar 

  • Suyana P, Sneha KR, Nair BN, Karunakaran V, Mohamed AP, KGK W, Hareesh US (2016) A facile one pot synthetic approach for C3N4-ZnS composite interfaces as heterojunctions for sunlight-induced multifunctional photocatalytic applications. RSC Adv 6:17800–17809

    Article  CAS  Google Scholar 

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

    Article  CAS  Google Scholar 

  • Wang X, Maeda K, Thomas A, Takanabe K, Xin G, Carlsson JM, Domen K, Antonietti M (2009) A metal-free polymeric photocatalyst for hydrogen production from water under visible light. Nat Mater 8:76–80

    Article  CAS  Google Scholar 

  • Wang X, Blechert S, Antonietti M (2012) Polymeric graphitic carbon nitride for heterogeneous photocatalysis. ACS Catal 2:1596–1606

    Article  Google Scholar 

  • Wu G, Li P, Xu D, Luo B, Hong Y, Shi W, Liu C (2015) Hydrothermal synthesis and visible-light-driven photocatalytic degradation for tetracycline of Mn-doped SrTiO3 nanocubes. Appl Surf Sci 333:39–47

    Article  CAS  Google Scholar 

  • Xu M, Han L, Dong S (2013) Facile fabrication of highly efficient g-C3N4/Ag2O heterostructured photocatalysts with enhanced visible-light photocatalytic activity. ACS Appl Mater Interfaces 5:12533–12540

    Article  CAS  Google Scholar 

  • Xue J, Ma S, Zhou Y, Zhang Z, He M (2015) Facile photochemical synthesis of Au/Pt/g-C3N4 with plasmon-enhanced photocatalytic activity for antibiotic degradation. ACS Appl Mater Interfaces 7:9630–9637

    Article  CAS  Google Scholar 

  • Yan M, Yan Y, Wu Y, Shi W, Hua Y (2015) Microwave-assisted synthesis of monoclinic-tetragonal BiVO4 heterojunctions with enhanced visible-light-driven photocatalytic degradation of tetracycline. RSC Adv 5:90255–90264

    Article  CAS  Google Scholar 

  • Yan Q, Xu M, Lin C, Hu J, Liu Y, Zhang R (2016) Efficient photocatalytic degradation of tetracycline hydrochloride by Ag3PO4 under visible-light irradiation. Environ Sci Pollut Res 23:14422–14430

    Article  CAS  Google Scholar 

  • Yan SC, Li ZS, Zou ZG (2009) Photodegradation performance of g-C3N4 fabricated by directly heating melamine. Langmuir 25:10397–10401

    Article  CAS  Google Scholar 

  • Ye L, Liu J, Jiang Z, Peng T, Zan L (2013) Facets coupling of BiOBr-g-C3N4 composite photocatalyst for enhanced visible-light-driven photocatalytic activity. Appl Catal B 142–143:1–7

    Google Scholar 

  • Ye S, Wang R, Wu M-Z, Yuan Y-P (2015) A review on g-C3N4 for photocatalytic water splitting and CO2 reduction. Appl Surf Sci 358(Part A):15–27

    Article  CAS  Google Scholar 

  • Zhang G, Zhang J, Zhang M, Wang X (2012a) Polycondensation of thiourea into carbon nitride semiconductors as visible light photocatalysts. J Mater Chem 22:8083–8091

    Article  CAS  Google Scholar 

  • Zhang J, Zhang M, Zhang G, Wang X (2012b) Synthesis of carbon nitride semiconductors in sulfur flux for water Photoredox catalysis. ACS Catal 2:940–948

    Article  CAS  Google Scholar 

  • Zhao Y, Zhang J, Qu L (2015) Graphitic carbon nitride/graphene hybrids as new active materials for energy conversion and storage. ChemNanoMat 1:298–318

    Article  CAS  Google Scholar 

  • Zhao YC, Yu DL, Zhou HW, Tian YJ, Yanagisawa O (2005) Turbostratic carbon nitride prepared by pyrolysis of melamine. J Mater Sci 40:2645–2647

Download references

Acknowledgements

Mr. Kiran Mohan is thankfully acknowledged for the HRTEM micrographs. The authors are grateful to the Council of Scientific and Industrial Research (CSIR, Government of India) for the 12th 5-year plan project on “IntelCoat” (CSC0114). Author S P thanks CSIR for the research fellowship.

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to Unnikrishnan Nair Saraswathy Hareesh.

Additional information

Responsible editor: Suresh Pillai

Electronic supplementary material

ESM 1

Detailed experimental method, characterization procedures, and EDX pattern of C3N4 is provided in the supporting information. (DOCX 82 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Panneri, S., Ganguly, P., Nair, B.N. et al. Role of precursors on the photophysical properties of carbon nitride and its application for antibiotic degradation. Environ Sci Pollut Res 24, 8609–8618 (2017). https://doi.org/10.1007/s11356-017-8538-z

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-017-8538-z

Keywords

Navigation