Abstract
Heterogeneous catalysis is widely known as an efficient, clean, and low-cost technology to mitigate the environmental pollution of industrial effluents. This research aimed at optimizing the preparation and characterization of efficient g-C3N4/Co3O4 nanocomposite for catalytic removal of Rhodamine B (Rh B) dye. The detected XRD peaks for the prepared nano-Co3O4 are matched with the cubic crystal structure. In contrast, the broad peak at 27.3° corresponding to the graphite reflection of hkl (002) was noticeably weakened in the XRD pattern of the g-C3N4/Co3O4 composite. FTIR spectra of g-C3N4/Co3O4 nanocomposites revealed the active vibrational modes of each Co3O4 and g-C3N4 component. The microstructure study of g-C3N4 showed the strong interlayer stacking of carbon nitride nanosheets, while the surface morphology of g-C3N4/Co3O4 nanocomposite revealed a hybrid particulate system. EDS analysis indicated that the spot area of g-C3N4/Co3O4 confirmed the chemical ratios of carbon, nitrogen, cobalt, and oxygen. BET measurements of g-C3N4/Co3O4 showed a significant increase in the surface area and pore volume of single components due to the lamination of stacked g-C3N4 nanosheets by the intercalated Co3O4 nanoparticles. The prepared 30% g-C3N4/Co3O4 revealed the lowest value of Eg ~1.2 eV and the highest light absorptivity suggesting strong promotion for the photocatalytic performance under visible light. The maximum photocatalytic activity of about 87% was achieved by 30% g-C3N4/Co3O4 due to the photonic enhancement, which reduces the recombination of excited electrons. The developed nanocomposite with a g-C3N4/Co3O4 ratio of 0.3 exhibited high stability in its photocatalytic performance after four recycling times, and a slight decrease of about 7% was estimated after the 5th reuse test.
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References
Aadil M, Zulfiqar S, Sabeeh H et al (2020) Enhanced electrochemical energy storage properties of carbon coated Co3O4 nanoparticles-reduced graphene oxide ternary nano-hybrids. Ceram Int 46:17836–17845. https://doi.org/10.1016/j.ceramint.2020.04.090
Ahmed SI, Sanad MMS (2021) Maghemite-based anode materials for Li-Ion batteries: the role of intentionally incorporated vacancies and cation distribution in electrochemical energy storage. J Alloys Compd 861:157962. https://doi.org/10.1016/j.jallcom.2020.157962
Alharthi FA, Alghamdi AA, Alanazi HS et al (2020) Photocatalytic degradation of the light sensitive organic dyes: methylene blue and rose bengal by using urea derived g-c3n4/zno nanocomposites. Catalysts 10:1–16. https://doi.org/10.3390/catal10121457
Bajdich M, García-Mota M, Vojvodic A et al (2013) Theoretical investigation of the activity of cobalt oxides for the electrochemical oxidation of water. J Am Chem Soc 135:13521–13530. https://doi.org/10.1021/ja405997s
Bankole OM, Olaseni SE, Adeyemo MA, Ogunlaja AS (2020) Microwave-assisted synthesis of cobalt oxide/reduced graphene oxide (Co3O4-RGO) composite and its sulfite enhanced photocatalytic degradation of organic dyes. Zeitschrift fur Phys Chemie 234(10):1681–1708. https://doi.org/10.1515/zpch-2019-1524
Bao EP, Dong R, Zhang S et al (2021) A Tubular g-C3N4 based composite photocatalyst combined with Co3O4 nanoparticles for photocatalytic degradation of diesel oil. Catal Lett 151:3437–3450. https://doi.org/10.1007/s10562-021-03583-y
Calza P, Minella M, Demarchis L et al (2020) Photocatalytic rate dependence on light absorption properties of different TiO2 specimens. Catal Today 340:12–18. https://doi.org/10.1016/j.cattod.2018.10.013
Chen F, Yang Q, Wang S, Yao F, Sun J, Wang Y, Zhang C, Li X, Niu C, Wang D, Zeng G (2017) Graphene oxide and carbon nitride nanosheets co-modified silver chromate nanoparticles with enhanced visible-light photoactivity and anti-photocorrosion properties towards multiple refractory pollutants degradation. Appl Catal B Environ 209:493–505
Dahal N, Ibarra IA, Humphrey SM (2012) High surface area mesoporous Co 3O 4 from a direct soft template route. J Mater Chem 22:12675–12681. https://doi.org/10.1039/c2jm30460k
Danish MSS, Estrella LL, Alemaida IMA et al (2021) Photocatalytic applications of metal oxides for sustainable environmental remediation. Metals 11:80. https://doi.org/10.3390/met11010080
Dhas CR, Venkatesh R, Jothivenkatachalam K, Nithya A, Benjamin BS, Raj AME, ... Sanjeeviraja C (2015) Visible light driven photocatalytic degradation of Rhodamine B and Direct Red using cobalt oxide nanoparticles. Ceram Int 41(8):9301–9313
Edla R, Patel N, Orlandi M et al (2015) Highly photo-catalytically active hierarchical 3D porous/urchin nanostructured Co3O4 coating synthesized by pulsed laser deposition. Appl Catal B Environ 166–167:475–484. https://doi.org/10.1016/j.apcatb.2014.11.060
Farhadi S, Safabakhsh J, Zaringhadam P (2013) Synthesis, characterization, and investigation of optical and magnetic properties of cobalt oxide (Co3O4) nanoparticles. Journal of Nanostructure in Chemistry 3:69. https://doi.org/10.1186/2193-8865-3-69
Feckl JM, Dunn HK, Zehetmaier PM et al (2015) Ultrasmall Co3O4 nanocrystals strongly enhance solar water splitting on mesoporous hematite. Adv Mater Interfaces 2:1–8. https://doi.org/10.1002/admi.201500358
Gasparotto A, Barreca D, Bekermann D et al (2011) F-doped Co 3 O 4 photocatalysts for sustainable H 2 generation from water/ethanol. J Am Chem Soc 133:19362–19365. https://doi.org/10.1021/ja210078d
Ge J, Zhang Y, Park SJ (2019) Recent advances in carbonaceous photocatalysts with enhanced photocatalytic performances: a mini review. Materials 12:1916
Han C, Ge L, Chen C et al (2014) Novel visible light induced Co3O4-g-C3N4 heterojunction photocatalysts for efficient degradation of methyl orange. Appl Catal B Environ 147:546–553. https://doi.org/10.1016/j.apcatb.2013.09.038
Hayat A, Sohail M, Taha TA et al (2021a) A butterfly shaped organic heterojunction photocatalyst for effective photocatalytic CO2reduction. CrystEngComm 23:4963–4974. https://doi.org/10.1039/d1ce00405k
Hayat A, Sohail M, Taha TA et al (2021b) A superficial intramolecular alignment of carbon nitride through conjugated monomer for optimized photocatalytic CO2 reduction. Catalysts 11. https://doi.org/10.3390/catal11080935
Hayat A, Taha TA, Alenad AM et al (2021c) A molecular amalgamation of carbon nitride polymer as emphasized photocatalytic performance. Int J Energy Res 45:19921–19928. https://doi.org/10.1002/er.7063
Hayat A, Taha TAM, Alenad AM et al (2021d) Organic conjugation of polymeric carbon nitride for improved photocatalytic CO2 conversion and H2 fixation. Energ Technol 9. https://doi.org/10.1002/ente.202100091
He Y, Zhang L, Wang X et al (2014) Enhanced photodegradation activity of methyl orange over Z-scheme type MoO3-g-C3N4 composite under visible light irradiation. RSC Adv 4:13610–13619. https://doi.org/10.1039/c4ra00693c
Helal A, Harraz FA, Ismail AA et al (2017) Hydrothermal synthesis of novel heterostructured Fe2O3/Bi2S3 nanorods with enhanced photocatalytic activity under visible light. Appl Catal B Environ 213:18–27. https://doi.org/10.1016/j.apcatb.2017.05.009
Helal A, Harraz FA, Ismail AA (2021a) One-step synthesis of heterojunction Cr2O3 nanoparticles decorated Bi2S3 nanorods with enhanced photocatalytic activity for mineralization of organic pollutants. J Photochem Photobiol A Chem 419:113468. https://doi.org/10.1016/j.jphotochem.2021.113468
Helal A, Yu J, Eid AI et al (2021b) Influence of a hole inversion layer at the In2O3 / BiVO4 interface on the high-efficiency photocatalytic performance. Surfaces and Interfaces 25:101148. https://doi.org/10.1016/j.surfin.2021.101148
Helal A, Jianqiang Y, Eid AI et al (2022) A novel g-C3N4/In2O3/BiVO4 heterojunction photoanode for improved the photoelectrochemical cathodic protection of 304 SS stainless steel under solar light. J Alloys Compd 911:165047. https://doi.org/10.1016/j.jallcom.2022.165047
Huang L, Li Y, Xu H et al (2013) Synthesis and characterization of CeO2/g-C3N 4 composites with enhanced visible-light photocatatalytic activity. RSC Adv 3:22269–22279. https://doi.org/10.1039/c3ra42712a
Jiménez-Salcedo M, Monge M, Tena MT (2021) The photocatalytic degradation of sodium diclofenac in different water matrices using g-C3N4 nanosheets: a study of the intermediate by-products and mechanism. J Environ Chem Eng 9:0–8. https://doi.org/10.1016/j.jece.2021.105827
Katsumata KI, Motoyoshi R, Matsushita N, Okada K (2013) Preparation of graphitic carbon nitride (g-C3N4)/WO3 composites and enhanced visible-light-driven photodegradation of acetaldehyde gas. J Hazard Mater 260:475–482. https://doi.org/10.1016/j.jhazmat.2013.05.058
Khan MW, Yao J, Zhang K et al (2019) Engineering N-reduced graphene oxide wrapped Co3O4@f-MWCNT hybrid for enhance performance dye-sensitized solar cells. J Electroanal Chem 844:142–154. https://doi.org/10.1016/j.jelechem.2019.05.008
Kumaravel S, Manoharan M, Haldorai Y, Rajendra Kumar RT (2022) Enhanced visible-light degradation of organic dyes via porous g-C3N4. Phosphorus Sulfur Silicon Relat Elem 197:200–208. https://doi.org/10.1080/10426507.2021.1991343
Li W, Jiang D, Yan P et al (2019) Graphitic carbon nitride/α-Fe2O3 heterostructures for sensitive photoelectrochemical non-enzymatic glucose sensor. Inorg Chem Commun 106:211–216. https://doi.org/10.1016/j.inoche.2019.06.015
Liu X, Jin A, Jia Y et al (2017) Synergy of adsorption and visible-light photocatalytic degradation of methylene blue by a bifunctional Z-scheme heterojunction of WO 3 /g-C 3 N 4. Appl Surf Sci 405:359–371. https://doi.org/10.1016/j.apsusc.2017.02.025
Liu H, Zhang ZG, He HW, Wang XX, Zhang J, Zhang QQ, Tong YF, Liu HL, Ramakrishna S, Yan SY, Long YZ (2018) One-step synthesis heterostructured g-CN/TiO composite for rapid degradation of pollutants in utilizing visible light. Nanomaterials (Basel, Switzerland) 8(10):842. https://doi.org/10.3390/nano8100842
Mahmoud MHH, Ismail AA, Sanad MMS (2012) Developing a cost-effective synthesis of active iron oxide doped titania photocatalysts loaded with palladium, platinum or silver nanoparticles. Chem Eng J 187:96–103. https://doi.org/10.1016/j.cej.2012.01.105
Mousavi M, Habibi-Yangjeh A (2017) Novel magnetically separable g-C3N4/Fe3O4/Ag3PO4/Co3O4 nanocomposites: visible-light-driven photocatalysts with highly enhanced activity. Adv Powder Technol 28:1540–1553. https://doi.org/10.1016/j.apt.2017.03.025
Naveen AN, Selladurai S (2014) Investigation on physiochemical properties of Mn substituted spinel cobalt oxide for supercapacitor applications. Electrochim Acta 125:404–414. https://doi.org/10.1016/j.electacta.2014.01.161
Nemiwal M, Zhang TC, Kumar D (2021) Recent progress in g-C3N4, TiO2 and ZnO based photocatalysts for dye degradation: strategies to improve photocatalytic activity. Sci Total Environ 767:144896
Paul DR, Gautam S, Panchal P et al (2020) ZnO-Modified g-C3N4: a potential photocatalyst for environmental application. ACS Omega 5:3828–3838. https://doi.org/10.1021/acsomega.9b02688
Raza SA, Naqvi SQ, Usman A et al (2021) Spectroscopic study of the interaction between rhodamine B and graphene. J Photochem Photobiol A Chem 418:113417. https://doi.org/10.1016/j.jphotochem.2021.113417
Sanad MMS, Farahat MM, El-Hout SI, El-Sheikh SM (2021) Preparation and characterization of magnetic photocatalyst from the banded iron formation for effective photodegradation of methylene blue under UV and visible illumination. J Environ Chem Eng 9. https://doi.org/10.1016/j.jece.2021.105127
Sanad MMS, El-Sadek MH (2022) Porous niobium carbide as promising anode for high performance lithium-ions batteries via cost-effective processing. Diam Relat Mater 121:108722. https://doi.org/10.1016/j.diamond.2021.108722
Sanad MMS, Rashad MM, Powers K (2015) Enhancement of the electrochemical performance of hydrothermally prepared anatase nanoparticles for optimal use as high capacity anode materials in lithium ion batteries (LIBs). Appl Phys Mater Sci Process 118:665–674. https://doi.org/10.1007/s00339-014-8776-6
Sanad MMS, Rashad MM, Shenouda AY (2016) Novel CuIn1-xGaxTe2 structures for high efficiency photoelectrochemical solar cells. Int J Electrochem Sci 11:4337–4351. https://doi.org/10.20964/2016.06.48
Shafiee MRM, Parhizkar J, Radfar S (2019) Removal of Rhodamine B by g-C3N4/Co3O4/MWCNT composite stabilized in hydrogel via the synergy of adsorption and photocatalysis under visible light. J Mater Sci Mater Electron 30(13):12475–12486
Soni V, Singh P, Khan AAP et al (2022) Photocatalytic transition-metal-oxides-based p–n heterojunction materials: synthesis, sustainable energy and environmental applications, and perspectives. J Nanostructure Chem 13:1–38
Sutar RS, Barkul RP, Delekar SD, Patil MK (2020) Sunlight assisted photocatalytic degradation of organic pollutants using g-C3N4-TiO2 nanocomposites. Arab J Chem 13:4966–4977. https://doi.org/10.1016/j.arabjc.2020.01.019
Taha TA, Saad SA (2020) Processing, thermal and dielectric investigations of polyester nanocomposites based on nano-CoFe2O4. Mater Chem Phys 255:123574. https://doi.org/10.1016/j.matchemphys.2020.123574
Tahir M, Mahmood N, Pan L et al (2016) Efficient water oxidation through strongly coupled graphitic C3N4 coated cobalt hydroxide nanowires. J Mater Chem A 4:12940–12946. https://doi.org/10.1039/c6ta05088c
Tauc J, Grigorovici R, Vancu A (1966) Optical properties and electronic structure of amorphous germanium. Phys Status Solidi B 15:627–637. https://doi.org/10.1002/pssb.19660150224
Thomas A, Fischer A, Goettmann F et al (2008) Graphitic carbon nitride materials: variation of structure and morphology and their use as metal-free catalysts. J Mater Chem 18:4893–4908. https://doi.org/10.1039/b800274f
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. https://doi.org/10.1002/anie.201101182
Wang M, Wu Z, Dai L (2015) Graphitic carbon nitrides supported by nitrogen-doped graphene as efficient metal-free electrocatalysts for oxygen reduction. J Electroanal Chem 753:16–20. https://doi.org/10.1016/j.jelechem.2015.05.012
Wang S, Feng Y, Yu M et al (2017a) Confined catalysis in the g -C 3 N 4 /Pt(111) interface: feasible molecule intercalation, tunable molecule–metal interaction, and enhanced reaction activity of CO oxidation. ACS Appl Mater Interfaces 9:33267–33273. https://doi.org/10.1021/acsami.7b08665
Wang Y, Yu D, Wang W et al (2017b) Synthesizing Co3O4-BiVO4/g-C3N4 heterojunction composites for superior photocatalytic redox activity. Adv Powder Technol 28:1540–1553. https://doi.org/10.1016/j.apt.2017.03.025
Wang Y, Yin X, Shen H et al (2018) Co3O4@g-C3N4 supported on N-doped graphene as effective electrocatalyst for oxygen reduction reaction. Int J Hydrog Energy 43:20687–20695. https://doi.org/10.1016/j.ijhydene.2018.09.140
Wang M, Li Z, Tian L et al (2019) A facile synthesis of nano-layer structured g-C 3 N 4 with efficient organic degradation and hydrogen evolution using a MDN energetic material as the starting precursor. Int J Hydrog Energy 44:4102–4113. https://doi.org/10.1016/j.ijhydene.2018.12.171
Wu M, Yan JM, Zhang XW, Zhao M (2015) Synthesis of g-C 3 N 4 with heating acetic acid treated melamine and its photocatalytic activity for hydrogen evolution. In: Applied Surface Science. Elsevier B.V., pp 196–200
Wu H, Li C, Che H et al (2018) Decoration of mesoporous Co 3 O 4 nanospheres assembled by monocrystal nanodots on g-C 3 N 4 to construct Z-scheme system for improving photocatalytic performance. Appl Surf Sci 440:308–319. https://doi.org/10.1016/j.apsusc.2018.01.134
Xiao J, Xie Y, Nawaz F et al (2016) Super synergy between photocatalysis and ozonation using bulk g-C3N4 as catalyst: a potential sunlight/O3/g-C3N4 method for efficient water decontamination. Appl Catal B Environ 181:420–428. https://doi.org/10.1016/j.apcatb.2015.08.020
Xu Q, Zhao P, Shi YK, Li JS, You WS, Zhang LC, Sang XJ (2020) Preparation of a gC3N4/Co3O4/Ag2O ternary heterojunction nanocomposite and its photocatalytic activity and mechanism. New J Chem 44(16):6261–6268
Yan SC, Li ZS, Zou ZG (2010) Photodegradation of rhodamine B and methyl orange over boron-doped g-C 3N4 under visible light irradiation. Langmuir 26:3894–3901. https://doi.org/10.1021/la904023j
Yang H, Lv K, Zhu J et al (2017) Effect of mesoporous g-C 3 N 4 substrate on catalytic oxidation of CO over Co3O4. Appl Surf Sci 401:333–340. https://doi.org/10.1016/j.apsusc.2016.12.238
Yang L, Liu J, Yang L et al (2020) Co3O4 imbedded g-C3N4 heterojunction photocatalysts for visible-light-driven hydrogen evolution. Renew Energy 145:691–698. https://doi.org/10.1016/j.renene.2019.06.072
Yang X, Zhang L, Wang D et al (2021) Facile synthesis of nitrogen-defective g-C3N4for superior photocatalytic degradation of rhodamine B. RSC Adv 11:30503–30509. https://doi.org/10.1039/d1ra05535f
Yin H, Zhu J, Chen J et al (2018) PEG-templated assembling of Co3O4 nanosheets with nanoparticles for enhanced sensitive non-enzymatic glucose sensing performance. J Mater Sci Mater Electron 29:17305–17313. https://doi.org/10.1007/s10854-018-9825-2
Zhang L, He Y, Ye P et al (2013) Enhanced photodegradation activity of Rhodamine B by Co3O 4/Ag3VO4 under visible light irriadiation. Materials Science and Engineering B: Solid-State Materials for Advanced Technology 178:45–52. https://doi.org/10.1016/j.mseb.2012.10.011
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Moustafa M.S. Sanad: conceptualization; data curation; formal analysis; investigation; methodology; writing original draft; review and editing. Taha A. Taha: methodology; funding acquisition; writing original draft. Ahmed Helal: investigation; methodology; writing original draft; Review and editing. Mohamed H. Mahmoud: formal analysis, visualization.
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Sanad, M.M., Taha, T.A., Helal, A. et al. Rational optimization of g-C3N4/Co3O4 nanocomposite for enhanced photodegradation of Rhodamine B dye under visible light. Environ Sci Pollut Res 30, 60225–60239 (2023). https://doi.org/10.1007/s11356-023-26767-y
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DOI: https://doi.org/10.1007/s11356-023-26767-y