Skip to main content
SpringerLink
Log in

Titanium silicalite-1 grafted with carbon nitride as carrier for cerium oxide-catalyzed ozonation of carboxylic acid in water

  • Published:
Reaction Kinetics, Mechanisms and Catalysis Aims and scope Submit manuscript

Abstract

Humic acid (HA) can be rapidly decomposed in single ozonation (SOZ); however, it undergoes incomplete degradation and inefficiency in abatement of the total organic carbon (TOC) is observed. In this study, titanium silicalite-1 grafted with carbon nitride was used as a carrier for cerium oxide (Ce-O/C3N4@TS-1), and this catalyst led to more rapid and thorough decomposition of HA in water. The TOC removal efficiencies of HA solution were 20% in SOZ against 62% in catalytic ozonation (COZ) after 60 min of reaction. Furthermore, in order to investigate the reasons for increasing degree of mineralization, in this study, the catalytic effect of the catalyst toward ozonation of oxalic acid (OA) was also investigated. The results showed that Ce-O/C3N4@TS-1 not only presented a good catalytic activity, but also exhibited an excellent stability. The good activity was attributed to the presence of Ce redox pair (Ce3+/Ce4+) on its surface and generation of hydroxyl radicals which has a rapid reaction rate with OA. C3N4 provide a large scaffold for anchoring Ce-O, which was responsible for the favorable stability.

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

Access this article

Log in via an institution

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

Similar content being viewed by others

References

  1. Martins RC, Quinta-Ferreira RM (2009) Catalytic ozonation of phenolic acids over a Mn-Ce-O catalyst. Appl Catal B 90:268–277

    Article  CAS  Google Scholar 

  2. Thomas A, Fischer A, Goettmann F, Antonietti M, Mueller J-O, Schloegl 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 

  3. Wang AJ, Li H, Huang H, Qian ZS, Feng JJ (2016) Fluorescent graphene-like carbon nitrides: synthesis, properties and applications. J Mater Chem 4:8146–8160

    CAS  Google Scholar 

  4. Fu J, Tian Y, Chang B, Xi F, Dong X (2012) BiOBr-carbon nitride heterojunctions: synthesis, enhanced activity and photocatalytic mechanism. J Mater Chem 22:21159–21166

    Article  CAS  Google Scholar 

  5. Qu AL, Xu XM, Xie HL, Zhang YY, Li YY, Wang JX (2016) Effects of calcining temperature on photocatalysis of g-C3N4/TiO2 composites for hydrogen evolution from water. Mater Res 80:167–176

    CAS  Google Scholar 

  6. Wang Y, Wang X, Antonietti M (2012) Polymeric graphitic carbon nitride as a heterogeneous organocatalyst: from photochemistry to multipurpose catalysis to sustainable chemistry. Angew Chem Int Ed 51:68–89

    Article  CAS  Google Scholar 

  7. Sun L, Zhao X, Jia C-J, Zhou Y, Cheng X, Li P, Liu L, Fan W (2012) Enhanced visible-light photocatalytic activity of g-C3N4-ZnWO4 by fabricating a heterojunction: investigation based on experimental and theoretical studies. J Mater Chem 22:23428–23438

    Article  CAS  Google Scholar 

  8. Wang Y, Bai X, Pan C, He J, Zhu Y (2012) Enhancement of photocatalytic activity of Bi2WO6 hybridized with graphite-like C3N4. J Mater Chem 22:11568–11573

    Article  CAS  Google Scholar 

  9. Zhou X, Jin B, Li L, Peng F, Wang H, Yu H, Fang Y (2012) A carbon nitride/TiO2 nanotube array heterojunction visible-light photocatalyst: synthesis, characterization, and photoelectrochemical properties. J Mater Chem 22:17900–17905

    Article  CAS  Google Scholar 

  10. Bonino F, Damin A, Ricchiardi G, Ricci M, Spano G, D’Aloisio R, Zecchina A, Lamberti C, Prestipino C, Bordiga S (2004) Ti-peroxo species in the TS-1/H2O2/H2O system. J Phys Chem B 108:3573–3583

    Article  CAS  Google Scholar 

  11. Camblor MA, Corma A, Perezpariente J (1993) Infrared spectroscopic invistigation of titanum in zeolites-a new assignment of the 960 cm−1 band. J Chem Soc, Chem Commun 6:557–559

    Article  Google Scholar 

  12. Srinivas D, Manikandan P, Laha SC, Kumar R, Ratnasamy P (2003) Reactive oxo-titanium species in titanosilicate molecular sieves: EPR investigations and structure-activity correlations. J Catal 217:160–171

    CAS  Google Scholar 

  13. Chaudhari K, Srinivas D, Ratnasamy P (2001) Reactive oxygen species in titanosilicates TS-1 and TiMCM-41: an in situ EPR spectroscopic study. J Catal 203:25–32

    Article  CAS  Google Scholar 

  14. Wang XS, Guo XW, Li G (2002) Synthesis of titanium silicalite (TS-1) from the TPABr system and its catalytic properties for epoxidation of propylene. Catal Today 74:65–75

    Article  CAS  Google Scholar 

  15. Chen C, Han C, Wang P, Guo S, Yan G, Li QX (2016) Investigation on titanium silicalite ETS-4 catalyzed ozonation for chemicals in wastewater, exemplified with 4-chlorophenol. Clean-Soil Air Water 44:1644–1651

    Article  CAS  Google Scholar 

  16. Soares OSGP, Rocha RP, Goncalves AG, Figueiredo JL, Orfao JJM, Pereira MFR (2016) Highly active N-doped carbon nanotubes prepared by an easy ball milling method for advanced oxidation processes. Appl Catal B 192:296–303

    Article  CAS  Google Scholar 

  17. Mitoraj D, Kisch H (2008) The nature of nitrogen-modified titanium dioxide photocatalysts active in visible light. Angew Chem Int Ed 47:9975–9978

    Article  CAS  Google Scholar 

  18. Brooks AC, France L, Gayot C, Li JPH, Sault R, Stafford A, Wallis JD, Stockenhuber M (2012) A designed organic-zeolite hybrid acid-base catalyst. J Catal 285:10–18

    Article  CAS  Google Scholar 

  19. Qin H, Chen H, Zhang X, Yang G, Feng Y (2014) Efficient degradation of fulvic acids in water by catalytic ozonation with CeO2/AC. J Chem Technol Biotechnol 89:1402–1409

    Article  CAS  Google Scholar 

  20. Faria PCC, Orfao JJM, Pereira MFR (2008) A novel ceria-activated carbon composite for the catalytic ozonation of carboxylic acids. Catal Commun 9:2121–2126

    Article  CAS  Google Scholar 

  21. Ding J, Qin Z, Zhang S (2014) Simultaneous desulfurization and denitrification of flue gas by catalytic ozonation over Ce-Ti catalyst. Fuel Process Technol 128:449–455

    Article  CAS  Google Scholar 

  22. Ding J, Qin Z, Zhang S (2015) A new insight into catalytic ozonation with nanosized Ce-Ti oxides for NOx removal: confirmation of Ce-O-Ti for active asites. Ind Eng Chem Res 54:2012–2022

    Article  CAS  Google Scholar 

  23. Gupta VK, Fakhri A, Agarwal S, Bharti AK, Naji M, Tkachev AG (2017) Preparation and characterization of TiO2 nanofibers by hydrothermal method for removal of benzodiazepines (diazepam) from liquids as catalytic ozonation and adsorption processes. J Mol Liq 249:1033–1038

    Article  CAS  Google Scholar 

  24. Liu J, Zhang T, Wang Z, Dawson G, Chen W (2011) Simple pyrolysis of urea into graphitic carbon nitride with recyclable adsorption and photocatalytic activity. J Mater Chem 21:14398–14401

    Article  CAS  Google Scholar 

  25. Xu J, Li Y, Peng S, Lu G, Li S (2013) Eosin Y-sensitized graphitic carbon nitride fabricated by heating urea for visible light photocatalytic hydrogen evolution: the effect of the pyrolysis temperature of urea. Phys Chem Chem Phys 15:7657–7665

    Article  CAS  PubMed  Google Scholar 

  26. Mitoraj D, Kisch H (2008) The nature of nitrogen-modified titanium dioxide photocatalysts pctive in visible light. Angew Chem Int Ed 47:9975–9978

    Article  CAS  Google Scholar 

  27. Li H, Lei Q, Zhang X, Suo J (2011) Nitrogen-incorporated TS-1 zeolite obtained by post-synthetic nitridation. Chemcatchem 3:143–145

    Article  CAS  Google Scholar 

  28. Gomes J, Costa R, Quinta-Ferreira RM, Martins RC (2017) Application of ozonation for pharmaceuticals and personal care products removal from water. Sci Total Environ 586:265–283

    Article  CAS  PubMed  Google Scholar 

  29. Faria PCC, Orfao JJM, Pereira MFR (2008) Catalytic ozonation of sulfonated aromatic compounds in the presence of activated carbon. Appl Catal B 83:150–159

    Article  CAS  Google Scholar 

  30. Faria PCC, Orfao JJM, Pereira MFR (2008) Activated carbon catalytic ozonation of oxamic and oxalic acids. Appl Catal B 79:237–243

    Article  CAS  Google Scholar 

  31. Shahidi D, Roy R, Azzouz A (2015) Advances in catalytic oxidation of organic pollutants—Prospects for thorough mineralization by natural clay catalysts. Appl Catal B 174:277–292

    Article  CAS  Google Scholar 

  32. Thurman EM, Malcolm RL (1981) Preparative isolation of aquatic humic substances. Environ Sci Technol 15:463–466

    Article  CAS  PubMed  Google Scholar 

  33. Liu J, Zhang T, Wang Z, Dawson G, Chen W (2011) Simple pyrolysis of urea into graphitic carbon nitride with recyclable adsorption and photocatalytic activity. J Mater Chem 21:14398–14401

    Article  CAS  Google Scholar 

  34. Gomes JF, Bednarczyk K, Gmurek M, Stelmachowski M, Zaleska-Medynska A, Bastos FC, Quinta-Ferreira ME, Costa R, Quinta-Ferreira RM, Martins RC (2017) Noble metal–TiO2 supported catalysts for the catalytic ozonation of parabens mixtures. Process Saf Environ Prot 111:148–159

    Article  CAS  Google Scholar 

  35. Yu L, Zhong Q, Deng Z, Zhang S (2016) Enhanced NOx removal performance of amorphous Ce-Ti catalyst by hydrogen pretreatment. J Mol Catal A 423:371–378

    Article  CAS  Google Scholar 

  36. Shao CY, Xu WB, Ollier N, Guzik M, Boulon G, Yu L, Zhang L, Yu CL, Wang SK, Hu LL (2016) Suppression mechanism of radiation-induced darkening by Ce doping in Al/Yb/Ce-doped silica glasses: evidence from optical spectroscopy, EPR and XPS analyses. J Appl Phys 120:153101–153108

    Article  CAS  Google Scholar 

  37. Matheswaran M, Balaji S, Chung SJ, Moon IS (2007) Studies on cerium oxidation in catalytic ozonation process: a novel approach for organic mineralization. Catal Commun 8:1497–1501

    Article  CAS  Google Scholar 

  38. Zhao H, Dong YM, Wang GL (2013) Novel magnetically separable nanomaterials for heterogeneous catalytic ozonation of phenol pollutant: NiFe2O4 and their performances. Chem Eng J 219:295–302

    Article  CAS  Google Scholar 

Download references

Author information

Authors and Affiliations

  1. Chengdu Institute of Organic Chemistry, Chinese Academy of Sciences, Chengdu, 610041, People’s Republic of China

    Jing Feng & Honglin Chen

  2. University of Chinese Academy of Sciences, Beijing, 100049, People’s Republic of China

    Jing Feng

Authors
  1. Jing Feng
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Honglin Chen
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Honglin Chen.

Electronic supplementary material

Below is the link to the electronic supplementary material.

Supplementary material 1 (DOCX 168 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Feng, J., Chen, H. Titanium silicalite-1 grafted with carbon nitride as carrier for cerium oxide-catalyzed ozonation of carboxylic acid in water. Reac Kinet Mech Cat 125, 339–350 (2018). https://doi.org/10.1007/s11144-018-1393-1

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11144-018-1393-1

Keywords

Search

Navigation