Abstract
In this work, we have fabricated a novel Fenton-like ferrihydrite/MoS2 (Fh/MoS2) composite and verified that the introduction of a small amount of iron on the surface of MoS2 can directly promote the exposure of Mo4+, finally enhancing the catalytic activity of the catalyst. Even though the content of iron element is only 1.19% in the composite, the reaction rate constant of Fh/MoS2 system for the degradation of environmental pollutants, such as organic dyes, antibiotic, and ionic liquid, is all much better than that of pure MoS2 system, which is attributed to much more generation of reactive oxygen species derived from synergistic effect of Fe3+/Fe2+ and Mo4+/Mo6+ redox cycles. The results of XPS and low-temperature EPR confirm that the exposure amount of Mo4+ active sites of 10% Fh/MoS2 is greatly increased, which is conducive to the conversion of Fe3+ to Fe2+ in the reaction process, thus effectively promoting the activation of H2O2.
Similar content being viewed by others
Data Availability
All data generated or analyzed during this study are included in this published article.
References
Afshar LE, Chaibakhsh N, Moradi-Shoeili Z (2018) Treatment of wastewater containing cytotoxic drugs by CoFe2O4 nanoparticles in Fenton/ozone oxidation process. Sep Sci Technol 53(16):2671–2682. https://doi.org/10.1080/01496395.2018.1461113
Barreiro JC, Capelato MD, Martin-Neto L, Hansen HCB (2007) Oxidative decomposition of atrazine by a Fenton-like reaction in a H2O2/ferrihydrite system. Water Res 41(1):55–62. https://doi.org/10.1016/j.watres.2006.09.016
Bokare AD, Choi W (2014) Review of iron-free Fenton-like systems for activating H2O2 in advanced oxidation processes. J Hazard Mater 275:121–135. https://doi.org/10.1016/j.jhazmat.2014.04.054
Cheng, M., Lai, C., Liu, Y., Zeng, G. M., Huang, D. L., Zhang, C., . . . Xiong, W. P. (2018). Metal-organic frameworks for highly efficient heterogeneous Fenton-like catalysis. Coord Chem Rev, 368, 80-92. https://doi.org/10.1016/j.ccr.2018.04.012
Cheng ZY, Luo SY, Li XJ, Zhang S, Nguyen TT, Guo MH, Gao X (2021) Ultrasound-assisted heterogeneous Fenton-like process for methylene blue removal using magnetic MnFe2O4/biochar nanocomposite. Appl Surf Sci 566. https://doi.org/10.1016/j.apsusc.2021.150654
Dai, L.-Y., Li, B., Xu, H.-Y., Wang, W.-S., Zhang, S.-Q., Xu, Y., . . . Jin, L.-G. (2023). Magnetic nanoreactor Fe3O4@HNTs as heterogeneous Fenton-like catalyst for acid fuchsin degradation: efficiency, kinetics and mechanism. J Phys Chem Solid, 180, 111445. https://doi.org/10.1016/j.jpcs.2023.111445
Dalal C, Garg AK, Sonkar SK (2021) Carboxylic acid-terminated carbon nanoflakes for selective adsorption of water-soluble cationic dyes. ACS Appl Nano Mater 4(5):5611–5620. https://doi.org/10.1021/acsanm.1c01148
Dong L, Lin S, Yang L, Zhang JJ, Yang C, Yang D, Lu HB (2014) Spontaneous exfoliation and tailoring of MoS2 in mixed solvents. Chem Commun 50(100):15936–15939. https://doi.org/10.1039/c4cc07238c
Fang YY, Huang QZ, Liu PY, Shi JF, Xu G (2018) A facile dip-coating method for the preparation of separable MoS2 sponges and their high-efficient adsorption behaviors of Rhodamine B. Inorg Chem Front 5(4):827–834. https://doi.org/10.1039/c8qi00012c
Gao XQ, Qi J, Wan SH, Zhang W, Wang Q, Cao R (2018) Conductive molybdenum sulfide for efficient electrocatalytic hydrogen evolution. Small 14(48). https://doi.org/10.1002/smll.201803361
Hasan, M. N., Altaf, M. M., Khan, N. A., Khan, A. H., Khan, A. A., Ahmed, S., . . . Islam, S. (2021). Recent technologies for nutrient removal and recovery from wastewaters: a review. Chemosphere, 277, 14. https://doi.org/10.1016/j.chemosphere.2021.130328
Huang HW, Tu SC, Zeng C, Zhang TR, Reshak AH, Zhang YH (2017) Macroscopic polarization enhancement promoting photo- and piezoelectric-induced charge separation and molecular oxygen activation. Angew Chem Int Ed 56(39):11860–11864. https://doi.org/10.1002/anie.201706549
Huo, X. Q., Yi, H., Fu, Y. K., An, Z. W., Qin, L., Liu, X. G., . . . Lai, C. (2021). Porous graphitic carbon nitride nanomaterials for water treatment. Environ Sci Nano, 8(7), 1835-1862. https://doi.org/10.1039/d1en00171j
Jayabal S, Saranya G, Liu YQ, Geng DS, Meng XB (2019) Unravelling the synergy effects of defect-rich 1T-MoS2/carbon nanotubes for the hydrogen evolution reaction by experimental and calculational studies. Sustainable Energy Fuels 3(8):2100–2110. https://doi.org/10.1039/c9se00244h
Ji JH, Yan QY, Yin PC, Mine SY, Matsuoka M, Xing MY (2021) Defects on CoS2-x: tuning redox reactions for sustainable degradation of organic pollutants. Angew Chem Int Ed 60(6):2903–2908. https://doi.org/10.1002/anie.202013015
Jiang, S., Hu, Q., Xu, M. Y., Hu, S. J., Shi, X. C., Ding, R., . . . Zhang, T. (2020). Crystalline CdS/MoS2 shape-controlled by a bacterial cellulose scaffold for enhanced photocatalytic hydrogen evolution. Carbohydr Polym, 250, 10. https://doi.org/10.1016/j.carbpol.2020.116909
Johnston CP, Chrysochoou M (2016) Mechanisms of chromate, selenate, and sulfate adsorption on Al-substituted ferrihydrite: implications for ferrihydrite surface structure and reactivity. Environ Sci Technol 50(7):3589–3596. https://doi.org/10.1021/acs.est.5b05529
Kumar, R., Sahoo, S., Joanni, E., Singh, R. K., Yadav, R. M., Verma, R. K., . . . Matsuda, A. (2019). A review on synthesis of graphene, h-BN and MoS2 for energy storage applications: recent progress and perspectives. Nano Res, 12(11), 2655-2694. https://doi.org/10.1007/s12274-019-2467-8
Lee Y, Lee W (2010) Degradation of trichloroethylene by Fe(II) chelated with cross-linked chitosan in a modified Fenton reaction. J Hazard Mater 178(1-3):187–193. https://doi.org/10.1016/j.jhazmat.2010.01.062
Li B, Xu H-Y, Liu Y-L, Liu Y, Xu Y, Zhang S-Q (2023) Unveiling the structure–activity relationships of ofloxacin degradation by Co3O4-activated peroxymonosulfate: from microstructures to exposed facets. Chem Eng J 467:143396. https://doi.org/10.1016/j.cej.2023.143396
Liu, J., Dong, C. C., Deng, Y. X., Ji, J. H., Bao, S. Y., Chen, C. R., . . . Xing, M. Y. (2018). Molybdenum sulfide co-catalytic Fenton reaction for rapid and efficient inactivation of Escherichia colis. Water Res, 145, 312-320. https://doi.org/10.1016/j.watres.2018.08.039
Liu Q, Zhao JZ, Wang Y, Liu YM, Dong JT, Xia JX, Li HM (2021) The novel photo-Fenton-like few-layer MoS2/FeVO4 composite for improved degradation activity under visible light irradiation. Colloids Surf A Physicochem Eng Asp 623. https://doi.org/10.1016/j.colsurfa.2021.126721
Liu S, Ni CY, Su H, Liu H, Chen RF, Li P, Wei Y (2016) Exploring the critical dependence of the adsorption of various dyes on the degradation rate using a ferrihydrite surface under visible light. RSC Adv 6(37):30840–30845. https://doi.org/10.1039/c5ra23868d
Long MS, Wang P, Fang HH, Hu WD (2019) Progress, challenges, and opportunities for 2D material based photodetectors. Adv Funct Mater 29(19):28. https://doi.org/10.1002/adfm.201803807
Luo HW, Cheng Y, Zeng YF, Luo K, Pan XL (2020) Enhanced decomposition of H2O2 by molybdenum disul fide in a Fenton-like process for abatement of organic micropollutants. Sci Total Environ 732:9. https://doi.org/10.1016/j.scitotenv.2020.139335
Ma W, Yao BH, Zhang W, He YQ, Yu Y, Niu JF, Wang C (2018) A novel multi- flaw MoS2 nanosheet piezocatalyst with superhigh degradation efficiency for ciprofloxacin. Environ Sci Nano 5(12):2876–2887. https://doi.org/10.1039/c8en00944a
Mitsunobu S, Muramatsu C, Watanabe K, Sakata M (2013) Behavior of antimony(V) during the transformation of ferrihydrite and its environmental implications. Environ Sci Technol 47(17):9660–9667. https://doi.org/10.1021/es4010398
Qian XF, Wu YW, Kan M, Fang MY, Yue DT, Zeng J, Zhao YX (2018) FeOOH quantum dots coupled g-C3N4 for visible light driving photo- Fenton degradation of organic pollutants. Appl Catal B Environ 237:513–520. https://doi.org/10.1016/j.apcatb.2018.05.074
Qiang TT, Chen L, Xia YJ, Qin XT (2021) Dual modified MoS2/SnS2 photocatalyst with Z-scheme heterojunction and vacancies defects to achieve a superior performance in Cr (VI) reduction and dyes degradation. J Clean Prod 291:12. https://doi.org/10.1016/j.jclepro.2020.125213
Rout K, Mohapatra M, Anand S (2012) 2-Line ferrihydrite: synthesis, characterization and its adsorption behaviour for removal of Pb(II), Cd(II), Cu(II) and Zn(II) from aqueous solutions. Dalton Trans 41(11):3302–3312. https://doi.org/10.1039/c2dt11651k
Sahoo D, Kumar B, Sinha J, Ghosh S, Roy SS, Kaviraj B (2020) Cost effective liquid phase exfoliation of MoS2 nanosheets and photocatalytic activity for wastewater treatment enforced by visible light. Sci Rep 10(1):12. https://doi.org/10.1038/s41598-020-67683-2
Shen, K. L., Cui, Y., Zhang, O. G., Liu, M. Y., Huang, H. Y., Sha, X. F., . . . Wei, Y. (2020). Biomimetic preparation of MoS2-Fe3O4 MNPs as heterogeneous catalysts for the degradation of methylene blue. J Environ Chem Eng, 8(5), 11. https://doi.org/10.1016/j.jece.2020.104125
Sheng, B., Yang, F., Wang, Y. H., Wang, Z. H., Li, Q., Guo, Y. G., . . . Liu, J. S. (2019). Pivotal roles of MoS2 in boosting catalytic degradation of aqueous organic pollutants by Fe(II)/PMS. Chem Eng J, 375, 10. https://doi.org/10.1016/j.cej.2019.121989
Shi XG, Tian A, You JH, Yang H, Wang YZ, Xue XX (2018) Degradation of organic dyes by a new heterogeneous Fenton reagent - Fe2GeS4 nanoparticle. J Hazard Mater 353:182–189. https://doi.org/10.1016/j.jhazmat.2018.04.018
Song XM, Tian JY, Shi WX, Cui FY, Yuan YX (2020) Significant acceleration of Fe2+/peroxydisulfate oxidation towards sulfisoxazole by addition of MoS2. Environ Res 188. https://doi.org/10.1016/j.envres.2020.109692
Tian YS, Zhou MH, Pan YW, Du XD, Wang Q (2021) MoS2 as highly efficient co-catalyst enhancing the performance of Fe-0 based electro-Fenton process in degradation of sulfamethazine: approach and mechanism. Chem Eng J 403:11. https://doi.org/10.1016/j.cej.2020.126361
Tong MP, Liu FY, Dong QQ, Ma ZY, Liu W (2020) Magnetic Fe3O4-deposited flower-like MoS2 nanocomposites for the Fenton-like Escherichia coli disinfection and diclofenac degradation. J Hazard Mater 385(10). https://doi.org/10.1016/j.jhazmat.2019.121604
Tseng WJ, Chuang YC, Chen YA (2018) Mesoporous Fe3O4@Ag@TiO2 nanocomposite particles for magnetically recyclable photocatalysis and bactericide. Adv Powder Technol 29(3):664–671. https://doi.org/10.1016/j.apt.2017.12.008
Vorontsov AV (2019) Advancing Fenton and photo-Fenton water treatment through the catalyst design. J Hazard Mater 372:103–112. https://doi.org/10.1016/j.jhazmat.2018.04.033
Wang JL, Wang SZ (2020) Reactive species in advanced oxidation processes: formation, identification and reaction mechanism. Chem Eng J 401:19. https://doi.org/10.1016/j.cej.2020.126158
Wu, D. F., Jiang, J. T., Tian, N. N., Wang, M., Huang, J., Yu, D. Y., . . . Ye, P. (2021). Highly efficient heterogeneous photo-Fenton BiOCl/MIL-100(Fe) nanoscaled hybrid catalysts prepared by green one-step coprecipitation for degradation of organic contaminants. RSC Adv, 11(51), 32383-32393. https://doi.org/10.1039/d1ra06549a
Wu YH, Su MH, Chen JW, Xu ZP, Tang JF, Chang XY, Chen DY (2019) Superior adsorption of methyl orange by h-MoS2 microspheres: isotherm, kinetics, and thermodynamic studies. Dyes Pigments 170. https://doi.org/10.1016/j.dyepig.2019.107591
Wu YJ, Chen RF, Liu H, Wei Y, Wu D (2014) Photo-catalyzed p-nitrophenol degradation in aqueous dispersions of ferrihydrite and H2O2. J Nanosci Nanotechnol 14(9):7325–7332. https://doi.org/10.1166/jnn.2014.8979
Xin, S. S., Ma, B. R., Liu, G. C., Ma, X. M., Zhang, C. L., Ma, X. H., . . . Xin, Y. J. (2021). Enhanced heterogeneous photo-Fenton-like degradation of tetracycline over CuFeO2/biochar catalyst through accelerating electron transfer under visible light. J Environ Manage, 285, 13. https://doi.org/10.1016/j.jenvman.2021.112093
Xing, M. Y., Xu, W. J., Dong, C. C., Bai, Y. C., Zeng, J. B., Zhou, Y., . . . Yin, Y. D. (2018). Metal sulfides as excellent co-catalysts for H2O2 decomposition in advanced oxidation processes. Chem, 4(6), 1359-1372. https://doi.org/10.1016/j.chempr.2018.03.002
Xiong, C. Y., Ren, Q. F., Liu, X. Y., Jin, Z., Ding, Y., Zhu, H. T., . . . Chen, R. R. (2021). Fenton activity on RhB degradation of magnetic g-C3N4/diatomite/Fe3O4 composites. Appl Surf Sci, 543. https://doi.org/10.1016/j.apsusc.2020.148844
Xu TY, Zhu RL, Zhu GQ, Zhu JX, Liang XL, Zhu YP, He HP (2017) Mechanisms for the enhanced photo-Fenton activity of ferrihydrite modified with BiVO4 at neutral pH. Appl Catal B Environ 212:50–58. https://doi.org/10.1016/j.apcatb.2017.04.064
Xu, Z. X., Lu, J. C., Zheng, X. Y., Chen, B., Luo, Y. M., Tahir, M. N., . . . Pan, X. J. (2020). A critical review on the applications and potential risks of emerging MoS2 nanomaterials. J Hazard Mater, 399, 30. https://doi.org/10.1016/j.jhazmat.2020.123057
Yamaguchi R, Kurosu S, Suzuki M, Kawase Y (2018) Hydroxyl radical generation by zero-valent iron/Cu (ZVI/Cu) bimetallic catalyst in wastewater treatment: heterogeneous Fenton/Fenton-like reactions by Fenton reagents formed in-situ under oxic conditions. Chem Eng J 334:1537–1549. https://doi.org/10.1016/j.cej.2017.10.154
Yin XL, Li YW, Huang XH, Tian J, Meng H, Wu W (2020) Scalable and efficient extraction of two-dimensional MoS2 nanosheets from dispersions as a co-catalyst for enhancing Fenton reactions. J Mater Sci 55(29):14358–14372. https://doi.org/10.1007/s10853-020-04897-9
Yuan X-Q, Xu H-Y, Li B, Dai L-Y, Wang W-S, Li Y (2023) Fenton-like degradation of methyl orange over CeO2 loaded on porous Al2O3: catalyst preparation, efficiency and mechanism. J Phys Chem Solid 178:111314. https://doi.org/10.1016/j.jpcs.2023.111314
Zhang MH, Dong H, Zhao L, Wang DX, Meng D (2019) A review on Fenton process for organic wastewater treatment based on optimization perspective. Sci Total Environ 670:110–121. https://doi.org/10.1016/j.scitotenv.2019.03.180
Zhang YF, Niu JF, Xu JH (2020) Fe(II)-promoted activation of peroxymonosulfate by molybdenum disulfide for effective degradation of acetaminophen. Chem Eng J 381:8. https://doi.org/10.1016/j.cej.2019.122718
Zhang ZM, Wang YQ, Jiang F, Liu QJ, Lang D (2021) Co-catalytic effect of molybdenum disulfide on Fenton reaction for the degradation of Acid Orange 7 Dye: reaction mechanism, performance optimization, and toxicity evaluation. Environ Eng Sci. https://doi.org/10.1089/ees.2020.0231
Zhao, J. X., Yin, J. J., Zhong, J. L., Jiao, T. F., Bai, Z. H., Wang, S. F., . . . Peng, Q. M. (2020). Facile preparation of a self-assembled Artemia cyst shell–TiO2–MoS2 porous composite structure with highly efficient catalytic reduction of nitro compounds for wastewater treatment. Nanotechnology, 31(8), 9. https://doi.org/10.1088/1361-6528/ab53c1
Zhu LL, Ji JH, Liu J, Mine SY, Matsuoka M, Zhang JL, Xing MY (2020a) Designing 3D-MoS2 sponge as excellent cocatalysts in advanced oxidation processes for pollutant control. Angew Chem Int Ed 59(33):13968–13976. https://doi.org/10.1002/anie.202006059
Zhu, R. L., Zhu, Y. P., Xian, H. Y., Yan, L. X., Fu, H. Y., Zhu, G. Q., . . . He, H. P. (2020b). CNTs/ferrihydrite as a highly efficient heterogeneous Fenton catalyst for the degradation of bisphenol A: the important role of CNTs in accelerating Fe (III)/Fe(II) cycling. Appl Catal B Environ, 270, 10. https://doi.org/10.1016/j.apcatb.2020.118891
Zhu, Y., Zhu, R., Yan, L., Fu, H., Xi, Y., Zhou, H., . . . He, H. (2018). Visible-light Ag/AgBr/ferrihydrite catalyst with enhanced heterogeneous photo-Fenton reactivity via electron transfer from Ag/AgBr to ferrihydrite. Appl Catal Environ, 239, 280-289. https://doi.org/10.1016/j.apcatb.2018.08.025
Funding
This work was supported financially by Natural Science Foundation of Tianjin City (No. 20JCQNJC00670) and the Open Foundation of Key Laboratory of Industrial Ecology and Environmental Engineering, MOE (KLIEEE-18-07).
Author information
Authors and Affiliations
Contributions
All authors contributed to the study conception and design. Material preparation, data collection, and analysis were performed by Da Chang and Juanjuan Sun. The first draft of the manuscript was written by Da Chang, and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.
Corresponding author
Ethics declarations
Ethics approval
Not applicable.
Consent to participate
Not applicable.
Consent for publication
Not applicable.
Conflict of interest
The authors declare no competing interests.
Additional information
Responsible Editor: Ricardo A. Torres-Palma
Publisher’s Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary information
ESM 1
Supplementary data to this article can be found in the “Supporting material” file. (DOCX 9579 kb)
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Chang, D., Sun, J., Wang, C. et al. Construction of a novel ferrihydrite/MoS2 heterogeneous Fenton-like catalyst for efficient degradation of organic pollutants under neutral conditions. Environ Sci Pollut Res 30, 105742–105755 (2023). https://doi.org/10.1007/s11356-023-29776-z
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11356-023-29776-z