Abstract
The degradation and mineralization of phenol have been studied by means of photocatalysis process using UV light (λmax ≈ 365 nm). The investigated nanocompositephotocatalyst TiO2-Py(750) (SBET=16.58 m2.g− 1), with mixed phases of Anatase and Rutile (52.2/10.7), have been sol-gel synthetized and calcined at 750 °C using a decarbonatedpyrophyllite as layered clay and titanium (IV) t-butoxide, Ti(OCH2CH2CH2CH3)4as precursor. Best results were achieved with TiO2-Py(750), which showed great photo-activity than that of labe-made TiO2 ECT1023t and commercial TiO2AEROXIDE®P25. The influences of different operating parameters, like pH, H2O2 concentration, photocatalyst dose, on the photodegradation of phenol by UV/TiO2-Py(750) system were examined. The TiO2-Py(750) showed total degradation, detoxification and good TOC mineralization at optimum conditions (pH = 5, [H2O2] = 10 mmol.L− 1, m = 2 g.L− 1). The toxicity analysis was carriedout based on the inhibition of bioluminescence of the marine bacteria Vibrio fischeri. The title photocatalysts have been investigated by UV-Vis diffuse reflectance spectroscopy (UV-Vis DRS), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), Fourier-transformed infrared spectroscopy (FTIR) and BET specific surface area.
Similar content being viewed by others
Data Availability
The authors confirm that the data supporting the findings of this study are available within the published article.
References
Sanjini NS, Velmathi S (2015) Photocatalytic degradation of Rhodamine B by mesoporous Ti-KIT-6 under UV light and solar light irradiation. J Porous Mater 22:1549–1558
Fegousse A, El Gaidoumi A, Miyah Y, El Mountassir R, Lahrichi A (2019) Pineapple bark performance in dyes adsorption: optimization by the central composite design. J Chem :3017163. https://doi.org/10.1155/2019/3017163
Battas A, El Gaidoumi A, Ksakas A, Kherbeche A (2019) Adsorption study for the removal of nitrate from water using local clay. Sci World J :9529618. https://doi.org/10.1155/2019/9529618
Karimi-Maleh H, Ayati A, Ghanbari S, Orooji Y, Tanhaei B, Karimi F, Alizadeh M, Rouhi J, Fu L, Sillanpää M (2021) Recent advances in removal techniques of Cr(VI) toxic ion from aqueous solution: A comprehensive review. J Mol Liq 329:115062
Karimi-Maleh H, Ayati A, Davoodi R, Karimi F, Tanhaei B, Malekmohammadi S, Orooji Y, Fu L, Sillanpää M (2021) Recent advances in using of chitosan-based adsorbents for removal of pharmaceutical contaminants: A review. J Clean Prod 291:125880
Karimi-Maleh H, Ranjbari S, Tanhaei B, Ayati A, Orooji Y, Alizadeh M, Karimi F, Salmanpour S, Rouhi J, Sillanpää M, Sen F (2021) Novel 1-butyl-3-methylimidazolium bromide impregnated chitosan hydrogel beads nanostructure as an efficient nanobio-adsorbent for cationic dye removal, 195. Kinetic study, p 110809
Karimi-Maleh H, Kumar BG, Qin S, Rajendran J, Vadivel S, Durgalakshmi D, Gracia F, Soto-Moscoso M, Orooji Y, Karimi F (2020) Tuning of metal oxides photocatalytic performance using Ag nanoparticles integration. J Mol Liq 314:113588
Karimi-Maleh H, Shafieizadeh M, Opoku F, Taher MA, Muriithi Kiarii E, Govender PP, Ranjbari S, Rezapour M, Orooji Y (2020) The role of magnetite/graphene oxide nano-composite as a high-efficiency adsorbent for removal of phenazopyridine residues from water samples, an experimental/theoretical investigation. J Mol Liq 298:112040
Sohrabi S, Akhlaghian F (2016) Light expanded clay aggregate (LECA) as a support for TiO2, Fe/TiO2, and Cu/TiO2nanocrystallinephotocatalysts, a comparative study on the structure, morphology, and activity. J Iran Chem Soc 13:1785–1796
Uddin MT, Islam MS, Abedin MZ (2007) Adsorption of phenol from aqueous solution by water hyacinth ash. J Eng Appl Sci 2:11–17
Ahmaruzzaman M (2008) Adsorption of phenolic compounds on low-cost adsorbents: a review. Adv Colloid Interface Sci 143:48–67
Kale D, Thakur P (2015) Highly efficient photocatalytic degradation and mineralization of 4-nitrophenol by graphene decorated ZnO. J Porous Mater 22:797–806
Yamasaki H, Makihatal Y, Fukunaga K (2008) Preparation of crosslinkedβ-cyclodextrin polymer beads and their application as a sorbent for removal of phenol from wastewater. J Chem Technol Biotechnol 83:991–997
Okasha AY, Ibrahim GH (2010) Phenol removal from aqueous systems by sorption of using some local waste materials. EJEAF Che 9:796–807
Kumar SD, Subbaiah VM, Reddy AS, Krishnaiah A (2009) Biosorption of phenolic compounds from aqueous solutions onto chitosan–abrusprecatorius blended beads. J Chem Technol Biotechnol 84:972–981
Yan J, Jianping W, Jing B, Daoquan W, Zongding H (2006) Phenol biodegradation by the yeast Candida tropicalis in the presence of m-cresol. Biochem Eng J 29:227–234
Kumaran P, Paruchuri YL (1996) Kinetics of phenol biotransformation. Water Res 31:11–22
Li Z, Burt T, Bowman RS (2000) Sorption of ionizable organic solutes by surfactant-modified zeolite. Environ Sci Technol 34:3756–3760
Yapar S, Klahre P, Klumpp E (2004) Hydrotalcite as a Potential Sorbent for the Removal of 2, 4-Dichlorophenol. Turkish J Eng Env Sci 28:41–48
Akcay M (2004) Characterization and determination of the thermodynamic and kinetic properties of p-CP adsorption onto organophilicbentonite from aqueous solution. J Colloid Interf Sci 280:299–304
Hao OJ, Kim H, Chiang PC (2000) Decolorization of wastewater. Crit Rev Environ Sci Technol 30:449–505
Dianat S, Tangestaninejad S, Mirkhani V, Moghadam M, Mohammadpoor-Baltork I (2013) Preparation, characterization and photocatalytic properties of InVO4nanopowder and InVO4-TiO2nanocomposite toward degradation of azo dyes and formaldehyde under visible light and ultrasonic irradiation. J Iran Chem Soc 10:535–544
Mirkhani V, Tangestaninejad S, Moghadam M, Habibi MH, Rostami Vartooni A (2009) Photodegradation of aromatic amines by Ag-TiO2 photocatalyst. J Iran Chem Soc 6:800–807
Assi N, Tehrani MS, Azar PA, Husain SW (2017) Microwave–assisted sol-gel synthesis of Fe2.9O4/ZnO core/shell nanoparticles using ethylene glycol and its use in photocatalytic degradation of 2-nitrophenol. J Iran Chem Soc 14:221–232
Roostaei N, Tezel H (2004) Removal of phenol from aqueous solutions by adsorption. J Environ Manage 70:157–164
Loqman A, El Bali B, El Gaidoumi A, Boularbah A, Kherbeche A, Lützenkirchen J (2021) The first application of moroccan perlite as industrial dyes removal. Silicon. https://doi.org/10.1007/s12633-021-01056-w
Nagabushan S, Prakash Jai BS, Iyengar P (2011) Oxidation of Phenol, o-nitro Phenol, o-chloro Phenol and Trichloroethylene Present in Water Using Surfactant Immobilized Manganate and Impregnated Metal Cations. Silicon 3:13–26
Kim S-R, Ali I, Kim J-O (2019) Phenol degradation using an anodized graphene-doped TiO2 nanotube composite under visible light. App Surf Sci 477:71–78
Xiaotong Wang J, Zhou S, Zhao X, Chen Y, Yu (2018) Synergistic effect of adsorption and visible-light photocatalysis for organic pollutant removal over BiVO4/carbon sphere nanocomposites. App Surf Sci 453:394–404
Wang T, Zhang Yan-ling, Pan Jia-hao, Li Bing-rui, Wu Li-guang, Jiang Bo-qiong (2019) Hydrothermal reduction of commercial P25 photocatalysts to expand their visible-light response and enhance their performance for photodegrading phenol in high-salinity wastewater. App Surf Sci 480:896–904
Ma D, Zhong J, Li J, Burda C, Duan R (2019) Preparation and photocatalytic performance of MWCNTs/BiOCl: Evidence for the superoxide radical participation in the degradation mechanism of phenol. App Surf Sci 480:395–403
Hameed BH, Rahman AA (2008) Removal of phenol from aqueous solutions by adsorption onto activated carbon prepared from biomass material. J Hazard Mater 160:576–581.
Wu SZ, Li N, Zhang WD (2014) Attachment of ZnO nanoparticles onto layered double hydroxides microspheres for high performance photocatalysis. J Porous Mater 21:157–164
Mills A, Le Hunte S (1997) An overview of semiconductor photocatalysis. J Photochem Photobiol A Chem 108:1–35
Hoffmann MR, Martin ST, Choi W, Bahnemann DW (1995) Environmental applications of semiconductor photocatalysis. Chem Rev 95:69–96
Fox MA, Dulay MT (1993) Heterogeneous photocatalysis. Chem Rev 93:341–357
Herrmann JM, Matos J, Disdier J, Guillard C, Laine J, Malato S, Blanco J (1999) Solar photocatalytic degradation of 4-chlorophenol using the synergistic effect between titania and activated carbon in aqueous suspension,Catal. Today 54:255–265
Corma A, Garcia H (2004) Zeolite-based photocatalystsChem Commun 13:1443–1459
Aicha B, Mohamed S, Jocelyne MB, Benedicte L, Jean-Luc B, Abdelkader B (2018) Preparation of new microporous titanium pillared kenyaite. materials active for the photodegradation of methyl orange. J Porous Mater 25:801–812
Hsien KJ, Tsai WT, Su TY (2009) Preparation of diatomite-TiO2 composite for photodegradation of bisphenol-A in water. J Sol-Gel Sci Technol 51:63–69
Xu H, Sun S, Jiang S, Wang H, Zhang R, Liu Q (2018) Effect of pretreatment on microstructure and photocatalytic activity of kaolinite/TiO2 composite. J Sol-Gel Sci Technol 87:676–684
Meng X, Qian Z, Wang H, Gao X, Zhang S, Yang M (2008) Sol-gel immobilization of SiO2/TiO2 on hydrophobic clay and its removal of methyl orange from water. J Sol-Gel Sci Technol 46:195–200
Zhao X, Meng Y, Lu X, Li X (2013) Sol-gel synthesis and catalytic property of Ce1-xTixO2 nanocomposites supported on attapulgite clay. J Sol-Gel Sci Technol 66:22–30
Liu J, Zhang G (2014) Recent advances in synthesis and applications of clay-based photocatalysts: a review. Phys Chem Chem Phys 16:8178–8192
Perathoner S, Centi G (2010) Catalytic wastewater treatment using pillared clays. In: Gil A, Korili SA, Trujillano R, Vicente MA (eds) Pillared clays and related catalysts. Springer, New York, pp 167
Chmielarz L, Gil B, Kustrowski P, Piwowarska Z, Dudek B, Michalik M (2009) Montmorillonite-based porous clay heterostructures (PCHs) intercalated with silica-titania pillars, synthesis and characterization. J Solid State Chem 182:1094–1104
Belver C, Aranda P, Martín-Luengo MA, Ruiz-Hitzky E (2012) New silica/alumina-clay heterostructures, Properties as acid catalysts. Micropor Mesopor Mater 147:157–166
Zhang J, Yan J, Sheng J (2015) Dry grinding effect on pyrophyllite-quartz natural mixture and its influence on the structural alternation of pyrophyllite. Micron 71:1–6
Ford RG, Sparks DL (2000) The nature of Zn precipitates formed in the presence of pyrophyllite. Environ Sci Technol 34:2479–2483
Prasad M, Saxena S, Amritphale SS, Chandra N (2000) Kinetics and isotherms for aqueous lead adsorption by natural minerals. Ind Eng Chem Res 39:3034–3037
Scheidegger AM, Lamble GM, Sparks DL (1996) Investigation of Ni sorption on pyrophyllite, an XAFS study. Environ Sci Technol 30:548–554
Keren R, Sparks DL (1994) Effect of pH and ionic strength on boron adsorption by pyrophyllite. Soil Sci Soc Am J 58:1095–1100
Saxena S, Prasad M, Amritphale SS, Chandra N (2001) Adsorption of cyanide from aqueous solutions at pyrophyllite surface. Sep Purif Technol 24:263–270
El Gaidoumi A, Loqman A, ChaouniBenadallah A, El Bali B, Kherbeche A (2019) Co(II)-pyrophyllite as catalyst for phenol oxidative degradation: optimization study using response surface methodology. Waste Biomass Valor 10:1043–1051
El Gaidoumi A, Chaouni Benabdallah A, El Bali B, Kherbeche A (2018) Synthesis and characterization of zeolite HS using natural pyrophyllite as new clay source. Arab J Sci Eng 43:191–197
El Gaidoumi A, Doña-Rodríguez JM, PulidoMelián E, González-Díaz OM, El Bali B, Navío JA, Kherbeche A (2019) Mesoporouspyrophyllite-titaniananocomposites: synthesis and activity in phenol photocatalytic degradation. Res Chem Interm 45:333–353
El Gaidoumi A, Chaouni Benabdallah A, Lahrichi A, Kherbeche A (2015) Adsorption du phénol en milieu aqueux par unepyrophylliteMarocaine brute et traitée (Adsorption of phenol in aqueous medium by a raw and treated Moroccan pyrophyllite). J Mater Environ Sci 6:2247–2259
El Gaidoumi A, Doña-Rodríguez JM, PulidoMelián E, González-Díaz OM, Navío JA, El Bali B, Kherbeche A (2019) Catalytic efficiency of Cu-supported pyrophyllite in heterogeneous catalytic oxidation of phenol. Arab J Sci Eng 44:6313–6325
El Gaidoumi A, Doña Rodríguez JM, Pulido Melián E, González-Díaz OM, Navío Santos JA, El Bali B, Kherbeche A (2019) Synthesis of sol-gel pyrophyllite/TiO2heterostructures: Effect of calcinationtemperature and methanol washing onphotocatalytic activity. Surf Interfaces 14:19–25
Araña J, Doña-Rodríguez JM, Portillo-Carrizo D, Fernández-Rodríguez C, Pérez-Peña J, GonzalezDiaz O, Navio JA, Macias M (2010) Photocatalytic degradation of phenolic compounds with new TiO2 catalysts. Appl Catal B Environ 100:346–354
Seck EI, Doña-Rodríguez JM, Pulido Melián E, Fernández-Rodríguez C, González-Díaz OM, Portillo-Carrizo D, Pérez-Peña J (2013) Comparative study of nanocrystalline titanium dioxide obtained through sol-gel and sol-gel-hydrothermal synthesis. J Colloid Interface Sci 400:31–40
Seck EI, Doña-Rodríguez JM, Fernández-Rodríguez C, González-Díaz OM, Araña J, Pérez-Peña J (2012) Photocatalytic removal of 2,4-dichlorophenoxyacetic acid by using sol-gel synthesized nanocrystalline and commercial TiO2: Operational parameters optimization and toxicity studies. Appl Catal B Environ 125:28–34
González Sánchez OM, Araña J, González Díaz O, Herrera Melián JA, Doña Rodríguez JM, Pérez-Peña J (2004) Detoxification of the herbicide propanil by means of Fenton process and TiO2-photocatalysis. J Photochem Photobiol A Chem 291:34–43
Seck EI, Doña-Rodríguez JM, Fernández-Rodríguez C, González-Díaz OM, Araña J, Pérez-Peña J (2012) Photocatalytical removal of bentazon using commercial and sol-gel synthesized nanocrystalline TiO2: Operational parameters optimization and toxicity studies. Chem Eng J 203:52–62
Santiago DE, Doña-Rodríguez JM, Araña J, Fernández-Rodríguez C, González-Díaz O, Pérez-Peña J, Silva AMT (2013) Optimization of the degradation of imazalil by photocatalysis: Comparison between commercial and lab-madephotocatalysts. Appl Catal B Environ 138–139:391–400
Patterson AL (1939) The Scherrer formula for X-ray particle size determination. Phys Rev 56:978–983
Spurr RA, Myers H (1957) Quantitative analysis of anatase rutile mixtures with an X-ray diffractometer. Anal Chem 29:760–762
Rivera-Utrilla J, Bautista-Toledo I, Ferro-Garcia MA, Moreno-Castilla C (2001) Activated carbon surface modifications by adsorption on bacteria and their effect on aqueous lead adsorption. J Chem Technol Biotechnol 76:1209–1215
Eisenberg G (1943) Colorimetric determination of hydrogen peroxide. Ind Eng Chem Anal Ed 15:327–328
Wang T, Wei J, Shi H, Zhou M, Zhang Y, Chen Q, Zhang Z (2017) Preparation of electrospun Ag/TiO2 nanotubes with enhanced photocatalytic activity based on water/oil phase separation. Physica E 86:103–110
Bentayeb A, Amouric M, Olives J, Dekayir A, Nadiri A (2003) XRD and HRTEM characterization of pyrophyllite from Morocco and its possible applications. Appl Clay Sci 22:211–221
Li G, Zeng J, Luo J, Liu M, Jiang T, Qiu G (2014) Thermal transformation of pyrophyllite and alkali dissolution behavior of silicon. Appl Clay Sci 99:282–288
Erdemoğlu M, Erdemoğlu S, Sayılkan F, Akarsu M, Şener Ş, Sayılkan H (2004) Organo functional modified pyrophyllite: preparation, characterisation and Pb(II) ion adsorption property. Appl Clay Sci 27:41–52
Hamzah N, Nordinc NM, Nadzri AHA, Nik YA, Kassim MB, Yarmo MA (2012) Enhanced activity of Ru/TiO2 catalyst using bisupport, bentonite-TiO2 for hydrogenolysis of glycerol in aqueous media. Appl Catal A General 419–420:133–141
Zhao X, Li J, Zhang Y, Dong H, Qu J, Qi T (2015) Preparation of nanosizedanatase TiO2-coated illite composite pigments by Ti(SO4)2 hydrolysis. Powder Technol 271:262–269
X.Zhao J, Li Y, Liu Y, Zhang J, Qu T, Qi (2014) Preparation and mechanism of TiO2-coated illite composite pigments. Dyes Pigments 108:84–92
Gao L, Zhan X, Lu Y, Li J, Sun Q (2015) pH-dependent structure and wettability of TiO2-based wood surface. Mater Lett 142:217–220
Li J, Suyoulema W, Wang, Sarina (2009) A study of photodegradation of sulforhodamine B on Au-TiO2/bentoniteunder UV and visible light irradiation. Solid State Sci 11:2037–2043
Aranda P, Belver C, Ruiz-Hitzky E (2014) Inorganic heterostructured materials based on clay minerals. In: Drummy LF, Ogawa M, Aranda P (eds) Materials and clay minerals, CMS Workshop Lectures, vol 18, The Clay Minerals Society, Chantilly. https://doi.org/10.1346/CMS-WLS-18-2
Sing KSW, Williams RT (2004) The use of molecular probes for the characterization of nanoporous adsorbents. Part Part Syst Charact 21:71–79
Munuera G, Moreno F, Gonzalez F (1972) In: Anderson JS, Roberts MW, Stone FS (eds) Reactivity of solids. Chapman Hall, London, p 681
Munuera G, Moreno F, Gonzalez F (1972) Reactivity of solids. Chapman Hall, London
Dzwigaj S, Arrouvel C, Breysse M, Geantet C, Inoue S, Toulhoat H, Raybaud P (2005) DFT makes the morphologies of Anatase-TiO2 nanoparticles visible to IR spectroscopy. J Catal 236:245–250
Vittadini A, Selloni A, Rotzinger FP, Gratzel M (1998) Structure and energetics of water adsorbed at TiO2 anatase (101) and (001) surfaces. Phys Rev Lett 81:2954–2957
Arrouvel C, Digne M, Breysse M, Toulhoat H, Raybaud P (2004) Effects of morphology on surface hydroxyl concentration: a DFT comparison of anatase–TiO2 and γ-alumina catalytic supports. J Catal 222:152–166
Ahmed S, Rasul MG, Martens WN, Brown R, Hashib MA (2010) Heterogeneous photocatalytic degradation of phenols in wastewater: A review on current status and developments. Desalination 261:3–18
Agarwal B, Balomajumder C, Kumar Thakur P (2013) Simultaneous co-adsorptive removal of phenol and cyanide from binary solution using granular activated carbon. Chem Eng J 228:655–664
Boukhatem H, Khalaf H, Djouadi L, Gonzalez FV, Navarro RM, Santaballa JA, Canle M (2017) Photocatalytic activity of mont-La (6 %)-Cu0.6Cd0.4S catalyst for phenol degradation under near UV visible light irradiation. Appl Catal B Environ 211:114–125
Ku Y, Leu RM, Lee KC (1996) Decomposition of 2-chlorophenol in aqueous solution by UV irradiation with the presence of titanium dioxide. Water Res 30:2569–2578
Mohamed F, Abukhadra MR, Shaban M (2018) Removal of safranin dye from water using poly pyrrolenano fiber/Zn-Fe layered double hydroxide nanocomposite (Ppy NF/Zn-Fe LDH) of enhanced adsorption and photocatalytic properties. Sci Total Environ 640–641:352–363
Shaban M, Abukhadra MR, Hamd A, Amin RR, Abdel Khalek A (2017) Photocatalytic removal of Congo red dye using MCM-48/Ni23 composite synthesized based on silica gel extracted from rice husk ash; fabrication and application. J Environ Manag 204:189–199
Shaban M, Ashraf AM, Abukhadra MR (2018) TiO2Nanoribbons/carbon nanotubes composite with enhanced photocatalytic activity; fabrication, characterization, and application. Sci Rep 8:781. https://doi.org/10.1038/s41598-018-19172-w
Shaban M, Abukhadra MR, Ibrahim SS, Shahien MG (2017) Photocatalytic degradation and photo-Fenton oxidation of Congo red dye pollutants in water using natural chromite-response surface optimization. Appl Water Sci 7:4743–4756
Gonçalves MST, Oliveira-Campos AMF, Pinto EMMS, Plasência PMS, Queiroz MJRP (1999) Photochemical treatment of solutions of azo dyes containing TiO2. Chemosphere 39:781–786
Delvin HP, Harris IJ (1984) Mechanism of the oxidation of aqueous phenol with dissolved oxygen. Ind Chem Fundam 23:387–392
Duprez D, Delanoë J, Barbier J, Isnard P, Blanchard G (1996) Catalytic oxidation of organic compounds in aqueous media. Catal Today 29:317–322
Acknowledgements
The authors would thank the Innovation Center of Sidi Mohamed Ben Abdellah University of Fez and the National Center for Scientific and Technical Research of Rabat (Morocco), for all collaborations.
Author information
Authors and Affiliations
Contributions
El Gaidoumi, Arrahli and Loqman carried out all research works supervising by Kherbeche. Baragh and El Bali participated in the interpretation of results and corrections of language.
Corresponding author
Ethics declarations
Ethics Approval and Consent to Participate
Not applicable.
Consent for Publication
Not applicable.
Conflict of Interest
The authors declare that they have no competing interests.
Research Involving Human Participants and/or Animals
Not applicable.
Informed Consent
Not applicable.
Additional information
Publisher’s Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
About this article
Cite this article
El Gaidoumi, A., Arrahli, A., Loqman, A. et al. Efficient Sol-gel Nanocomposite TiO2-clay in Photodegradation of Phenol: Comparison to Labe-made and Commercial Photocatalysts. Silicon 14, 5401–5414 (2022). https://doi.org/10.1007/s12633-021-01275-1
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s12633-021-01275-1