Abstract
Semiconductor photocatalysis has been regarded as one of the most promising methods for treatment of Cr(VI)-containing wastewater, but the high recombination rate of photogenerated carriers and photocorrosion have limited severely its practical application. The objective of the current study was to employ a layered double hydroxide (LDH) to mitigate these problems by designing and constructing a multiple heterojunction system of g-C3N4/LDH/Ag3PO4 (CNLDHAP) through a two-step hydrothermal route. The structures, morphologies, chemical states, and optical properties of the products were investigated systematically. The CNLDHAP composite showed superior photocatalytic activity for Cr(VI) reduction than that of the individual components under visible-light irradiation. The composite exhibited high photocatalytic reduction stability after five recycles. The enhanced photocatalytic performance may originate from the very efficient separation of photogenerated carriers of the multiple heterojunction system. Possible photocatalytic mechanisms for the reduction of Cr(VI) over the CNLDHAP composite photocatalyst are proposed.
Similar content being viewed by others
REFERENCES
Abroshan, E., Farhadi, S., & Zabardasti, A. (2018). Novel magnetically separable Ag3PO4/MnFe2O4 nanocomposite and its high photocatalytic degradation performance for organic dyes under solar-light irradiation. Solar Energy Materials and Solar Cells, 178, 154–163.
Chen, C., Zeng, H., Xu, S., Liu, X., Duan, H., & Han, J. (2017). Preparation of mesoporous material from hydrotalcite/carbon composite precursor for chromium(VI) removal. Journal of the Taiwan Institute of Chemical Engineers, 70, 302–310.
Chen, C. R., Zeng, H. Y., Xu, S., Shen, J. C., Hu, G., Zhu, R. L., Du, J. Z., & Sun, Y. X. (2018). Facile fabrication of CdS/ZnAlO heterojunction with enhanced photocatalytic activity for Cr(VI) reduction under visible light. Applied Clay Science, 165, 197–204.
Chen, C., Zeng, H., Yi, M., Xiao, G., Xu, S., Shen, S., & Feng, B. (2019a). In-situ growth of Ag3PO4 on calcined Zn-Al layered double hydroxides for enhanced photocatalytic degradation of tetracycline under simulated solar light irradiation and toxicity assessment. Applied Catalysis B: Environmental, 252, 47–54.
Chen, C., Zeng, H., Yi, M., Xiao, G., Zhu, R., Cao, X., Shen, S., & Peng, J. (2019b). Fabrication of Ag2O/Ag decorated ZnAl-layered double hydroxide with enhanced visible light photocatalytic activity for tetracycline degradation. Ecotoxicology and Environmental Safety, 172, 423–431.
Das, S., Patnaik, S., & Parida, K. M. (2019). Fabrication of a Au-loaded CaFe2O4/CoAl LDH p–n junction based architecture with stoichiometric H2 & O2 generation and Cr(vi) reduction under visible light. Inorganic Chemistry Frontiers, 6, 94–109.
Dhanabal, R., Velmathi, S., & Chandra, A. (2018). Bose Fabrication of RuO2-Ag3PO4 heterostructure nanocomposites: Investigations of band alignment on the enhanced visible light photocatalytic activity. Journal of Hazardous Materials, 344, 865–874.
Fang, J., Li, M., Li, Q., Zhang, W., Shou, Q., Liu, F., Zhang, X., & Cheng, J. (2012). Microwave-assisted synthesis of CoAl-layered double hydroxide/graphene oxide composite and its application in supercapacitors. Electrochimica Acta, 85, 248–255.
Fettkenhauer, C., Clavel, G., Kailasam, K., Antonietti, M., & Dontsova, D. (2015). Facile synthesis of new, highly efficient SnO2/carbon nitride composite photocatalysts for the hydrogen evolution reaction. Green Chemistry, 17, 3350–3361.
Hu, J., Chen, D., Mo, Z., Li, N., Xu, Q., Li, H., He, J., Xu, H., & Lu, J. (2019). Z-Scheme 2D/2D Heterojunction of black phosphorus/monolayer Bi2WO6 nanosheets with enhanced photocatalytic activities. Angewandte Chemie, 131, 2095–2099.
Jing, F., Liang, R., Xiong, J., Chen, R., Zhang, S., Li, Y., & Wu, L. (2017). MIL-68(Fe) as an efficient visible-light-driven photocatalyst for the treatment of a simulated waste-water contain Cr(VI) and Malachite Green. Applied Catalysis B: Environmental, 206, 9–15.
Jo, W. K., & Tonda, S. (2019). Novel CoAl-LDH/g-C3N4/RGO ternary heterojunction with notable 2D/2D/2D configuration for highly efficient visible-light-induced photocatalytic elimination of dye and antibiotic pollutants. Journal of Hazardous Materials, 368, 778–787.
Kang, Q., Cao, J., Zhang, Y., Liu, L., Xu, H., & Ye, J. (2013). Reduced TiO2 nanotube arrays for photoelectrochemical water splitting. Journal of Materials Chemistry A, 1, 5766–5774.
Kumar, S., Surendar, T., Baruah, A., & Shanker, V. (2013). Synthesis of a novel and stable g-C3N4–Ag3PO4 hybrid nanocomposite photocatalyst and study of the photocatalytic activity under visible light irradiation. Journal of Materials Chemistry A, 1, 5333–5340.
Kumar, S., Isaacs, M. A., Trofimovaite, R., Durndell, L., Parlett, C. M. A., Douthwaite, R. E., Coulson, B., Cockett, M. C. R., Wilson, K., & Lee, A. F. (2017). P25@CoAl layered double hydroxide heterojunction nanocomposites for CO2 photocatalytic reduction. Applied Catalysis B: Environmental, 209, 394–404.
Li, H., Li, J., Xu, C., Yang, P., Ng, D. H. L., Song, P., & Zuo, M. (2017). Hierarchically porous MoS2/CoAl-LDH/HCF with synergistic adsorption-photocatalytic performance under visible light irradiation. Journal of Alloys and Compounds, 698, 852–862.
Li, K., Huang, Z., Zhu, S., Luo, S., Yan, L., Dai, Y., Guo, Y., & Yang, Y. (2019). Removal of Cr(VI) from water by a biochar-coupled g-C3N4 nanosheets composite and performance of a recycled photocatalyst in single and combined pollution systems. Applied Catalysis B: Environmental, 243, 386–396.
Liu, Y., Zhu, G., Gao, J., Hojamberdiev, M., Zhu, R., Wei, X., Guo, Q., & Liu, P. (2017). Enhanced photocatalytic activity of Bi4Ti3O12 nanosheets by Fe3+-doping and the addition of Au nanoparticles: photodegradation of phenol and bisphenol A. Applied Catalysis B: Environmental, 200, 72–82.
Liu, X., Xu, J., Ni, Z., Wang, R., You, J., & Guo, R. (2019a). Adsorption and visible-light-driven photocatalytic properties of Ag3PO4/WO3 composites: a discussion of the mechanism. Chemical Engineering Journal, 356, 22–33.
Liu, D., Chen, D., Li, N., Xu, Q., Li, H., He, J., & Lu, J. (2019). ZIF-67-Derived 3D Hollow Mesoporous crystalline Co3O4 wrapped by 2D g-C3N4 nanosheets for photocatalytic removal of nitric oxide. Small, 15, 1902291.
Luo, J., Luo, X., Crittenden, J., Qu, J., Bai, Y., Peng, Y., & Li, J. (2015). Removal of antimonite (Sb(III)) and antimonate (Sb(V)) from aqueous solution using carbon nanofibers that are decorated with zirconium oxide (ZrO2). Environmental Science & Technology, 49, 11115–11124.
Luo, J., Sun, M., Ritt, C. L., Liu, X., Pei, Y., Crittenden, J. C., & Elimelech, M. (2019). Tuning Pb(II) adsorption from aqueous solutions on ultrathin iron oxychloride (FeOCl) nanosheets. Environmental Science & Technology, 53, 2075–2085.
Ma, R., Liang, J., Takada, K., & Sasaki, T. (2010). Topochemical synthesis of Co-Fe layered double hydroxides at varied Fe/Co ratios: unique intercalation of triiodide and its profound effect. Journal of the American Chemical Society, 133, 613–620.
Nanda, B., Pradhan, A. C., & Parida, K. M. (2017). Fabrication of mesoporous CuO/ZrO2-MCM-41 nanocomposites for photocatalytic reduction of Cr(VI). Chemical Engineering Journal, 316, 1122–1135.
Peng, W., Li, H., & Song, S. (2017a). Synthesis of fluorinated graphene/CoAl-layered double hydroxide composites as electrode materials for supercapacitors. ACS Applied Materials & Interfaces, 9, 5204–5212.
Peng, W., Li, H., Liu, Y., & Song, S. (2017b). Effect of oxidation degree of graphene oxide on the electrochemical performance of CoAl-layered double hydroxide/graphene composites. Applied Materials Today, 7, 201–211.
Shakeel, M., Arif, M., Yasin, G., Li, B., & Khan, H. D. (2019). Layered by layered Ni-Mn-LDH/g-C3N4 nanohybrid for multi-purpose photo/electrocatalysis: Morphology controlled strategy for effective charge carriers separation. Applied Catalysis B: Environmental, 242, 485–498.
Shao, B., Liu, X., Liu, Z., Zeng, G., Liang, Q., Liang, C., Cheng, Y., Zhang, W., Liu, Y., & Gong, S. (2019). A novel double Z-scheme photocatalyst Ag3PO4/Bi2S3/Bi2O3 with enhanced visible-light photocatalytic performance for antibiotic degradation. Chemical Engineering Journal, 368, 730–745.
Sun, Q., Hu, X., Zheng, S., Zhang, J., & Sheng, J. (2019). Effect of calcination on structure and photocatalytic property of N-TiO2/g-C3N4@diatomite hybrid photocatalyst for improving reduction of Cr(VI). Environmental Pollution, 245, 53–62.
Tan, P., Chen, X., Wu, L., Shang, Y., Liu, W., Pan, J., & Xiong, X. (2017). Hierarchical flower-like SnSe2 supported Ag3PO4 nanoparticles: towards visible light driven photocatalyst with enhanced performance. Applied Catalysis B: Environmental, 202, 326–334.
Tian, L., Yang, X., Cui, X., Liu, Q., & Tang, H. (2019). Fabrication of dual direct Z-scheme g-C3N4/MoS2/Ag3PO4 photocatalyst and its oxygen evolution performance. Applied Surface Science, 463, 9–17.
Tonda, S., Kumar, S., Bhardwaj, M., Yadav, P., & Ogale, S. (2018). g-C3N4/NiAl-LDH 2D/2D hybrid heterojunction for high-performance photocatalytic reduction of CO2 into renewable fuels. ACS Applied Materials & Interfaces, 10, 2667–2678.
Velegraki, G., Miao, J., Drivas, C., Liu, B., Kennou, S., & Armatas, G. S. (2018). Fabrication of 3D mesoporous networks of assembled CoO nanoparticles for efficient photocatalytic reduction of aqueous Cr(VI). Applied Catalysis B: Environmental, 221, 635–644.
Wan, J., Du, X., Liu, E., Hu, Y., Fan, J., & Hu, X. (2017). Z-scheme visible-light-driven Ag3PO4 nanoparticle@MoS2 quantum dot/few-layered MoS2 nanosheet heterostructures with high efficiency and stability for photocatalytic selective oxidation. Journal of Catalysis, 345, 281–294.
Wang, S., Li, C., Wang, T., Zhang, P., Lia, A., & Gong, J. (2014). Controllable synthesis of nanotube-type graphitic C3N4 and their visible-light photocatalytic and fluorescent properties. Journal of Materials Chemistry A, 2, 2885–2890.
Wang, K., Zhang, L., Su, Y., Shao, D., Zeng, S., & Wang, W. (2018). Photoreduction of carbon dioxide of atmospheric concentration to methane with water over CoAl-layered double hydroxide nanosheets. Journal of Materials Chemistry A, 6, 8366–8373.
Wang, X., Liu, W., Fu, H., Yi, X., Wang, P., Zhao, C., Wang, C., & Zheng, W. (2019). Simultaneous Cr(VI) reduction and Cr(III) removal of bifunctional MOF/Titanate nanotube composites. Environmental Pollution, 249, 502–511.
Wu, J., Wang, J., Du, Y., Li, H., Yang, Y., & Jia, X. (2015). Chemically controlled growth of porous CeO2 nanotubes for Cr(VI) photoreduction. Applied Catalysis B: Environmental, 174, 435–444.
Wu, Y., Wang, H., Sun, Y., Xiao, T., Tu, W., Yuan, X., Zeng, G., Li, S., & Chew, J. W. (2018). Photogenerated charge transfer via interfacial internal electric field for significantly improved photocatalysis in direct Z-scheme oxygen-doped carbon nitrogen/CoAl-layered double hydroxide heterojunction. Applied Catalysis B: Environmental, 227, 530–540.
Xu, H., Wang, C., Song, Y., Zhu, J., Xu, Y., Yan, J., Song, Y., & Li, H. (2014). CNT/Ag3PO4 composites with highly enhanced visible light photocatalytic activity and stability. Chemical Engineering Journal, 241, 35–42.
Xu, T., Zhu, R., Zhu, G., Zhu, J., Liang, X., Zhu, Y., & He, H. (2017). Mechanisms for the enhanced photo-Fenton activity of ferrihydrite modified with BiVO4 at neutral pH. Applied Catalysis B: Environmental, 212, 50–58.
Yang, W., Li, J., Liu, M., Ng, D. H. L., Liu, Y., Sun, X., & Yang, J. (2019). Bioinspired hierarchical CoAl-LDH/MFe2O4 (Ni, Zn, Co) as peroxidase mimics for colorimetric detection of glucose. Applied Clay Science, 181, 105238–105249.
Yuan, R., Yue, C., Qiu, J., Liu, F., & Li, A. (2019). Highly efficient sunlight-driven reduction of Cr(VI) by TiO2@NH2-MIL-88B(Fe) heterostructures under neutral conditions. Applied Catalysis B: Environmental, 251, 229–239.
Zhang, L., Li, L., Sun, X., Liu, P., Yang, D., & Zhao, X. (2016a). ZnO-layered double hydroxide@graphitic carbon nitride composite for consecutive adsorption and photodegradation of dyes under UV and visible lights. Materials, 9, 927.
Zhang, S., Zhang, Y., Jiang, W., Liu, X., Xu, S., Huo, R., Zhang, F., & Hu, J. (2016b). Co@N-CNTs derived from triple-role CoAl-layered double hydroxide as an efficient catalyst for oxygen reduction reaction. Carbon, 107, 162–170.
Zhao, Y., Chen, G., Bian, T., Zhou, C., Waterhouse, G. I. N., Wu, L., Tung, C. H., Smith, L. J., O’Hare, D., & Zhang, T. (2015). Defect-rich ultrathin ZnAl-layered double hydroxide nanosheets for efficient photoreduction of CO2 to CO with water. Advanced Materials, 27, 7824–7831.
Zhao, Y., Jia, X., Waterhouse, G. I. N., Wu, L., Tung, C. H., O’Hare, D., & Zhang, T. (2016). Layered double hydroxide nanostructured photocatalysts for renewable energy production. Advanced Energy Materials, 6, 1501974.
Zheng, Y., Lin, L., Wang, B., & Wang, X. (2015). Graphitic carbon nitride polymers toward sustainable photoredox catalysis. Angewandte Chemie International Edition, 54, 12868–12884.
Zhong, Y., Qiu, X., Chen, D., Li, N., Xu, Q., Li, H., He, J., & Lu, J. (2016). Flexible electrospun carbon nanofiber/tin(IV) sulfide core/sheath membranes for photocatalytically treating chromium(VI)-containing wastewater. ACS Applied Materials & Interfaces, 8, 28671–28677.
Zhou, L., Zhang, W., Chen, L., & Deng, H. (2017). Z-scheme mechanism of photogenerated carriers for hybrid photocatalyst Ag3PO4/g-C3N4 in degradation of sulfamethoxazole. Journal of Colloid and Interface Science, 487, 410–417.
ACKNOWLEDGMENTS
This work was supported by the Key Research and Development Program of Hunan Province (2018SK20110).
Funding
Funding sources are as stated in the Acknowledgments.
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of Interest
The authors declare that they have no conflict of interest.
Additional information
(Received 16 September 2020; revised 8 March 2021; AE: Jun Kawamata)
Supplementary Information
Below is the link to the electronic supplementary material.
Rights and permissions
About this article
Cite this article
Chen, CR., Zeng, HY., Xiong, J. et al. MULTIPLE HIERARCHICAL HETEROJUNCTION g-C3N4/LDH/Ag3PO4 WITH ENHANCED VISIBLE-LIGHT PHOTOCATALYTIC ACTIVITY FOR Cr(VI) REDUCTION. Clays Clay Miner. 69, 243–253 (2021). https://doi.org/10.1007/s42860-021-00121-0
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s42860-021-00121-0