Journal of Particle Science and Technology

Journal of Particle Science and Technology

Adsorption of methylene blue on lithium titanate and its composite with carbon dots: Optimization of parameters and adsorbent recovery

Document Type : Research Article

Authors
Department of Chemistry, University of Sistan and Baluchestan, Zahedan, Iran
Abstract
Porous lithium-titanium oxide (pLT) was produced by the combustion synthesis method. Based on the XRD pattern, the as-synthesized powder phase was Li2TiO3. The carbon dots were incorporated onto the lithium titanate sponge (pLT-CD) using the microwave method and natural precursors. Two synthesized structures were used to remove methylene blue from wastewater. A morphological comparison of pLT and pLT-CD was performed using field emission scanning electron microscopy. Elemental mapping of the pLT-CD composite was used to investigate the dispersion of CD on pLT and its stability in aqueous media. The experiments of methylene blue removal by adsorbents were designed using the Taguchi method. The effect of pH, time, temperature, and methylene blue concentration on the treatment process by pLT and pLT-CD was studied. The maximum removal percentage was observed at pH 8, room temperature, 10 min, and 40 ppm dye concentration on the pLT-CD composite adsorbent. The adsorption equilibrium was better described by the Freundlich isotherm, indicating multilayer adsorption on heterogeneous surfaces. Kinetic results followed a pseudo-second-order model, with pLT-CD showing a higher adsorption rate due to enhanced surface interactions and increased active sites. Adsorbent recovery was performed by UV-Vis irradiation on the saturated adsorbent to decompose the adsorbed dye. An efficiency drop of about 20 and 13.60 % was observed for pLT and pLT-CD, respectively, after four consecutive cycles

Graphical Abstract

Adsorption of methylene blue on lithium titanate and its composite with carbon dots: Optimization of parameters and adsorbent recovery

Highlights

  • Fabrication and characterization of porous Li2TiO3(pLT)
  • Incorporation of carbon dots on Li2TiO3(pLT-CD)
  • Analysis of the adsorption of methylene blue on pLT and pLT-CD
  • Optimization of adsorption parameters

Keywords
Subjects

Copyright © 2025 The Author(s). Published by IROST.

[1]  Wong, S., Ghafar, N. A., Ngadi, N., Razmi, F. A., Inuwa, I. M., Mat, R., & Amin, N. A. (2020). Effective Removal of Anionic Textile Dyes Using Adsorbent Synthesized from Coffee Waste. Scientific Reports, 10, 2928. https://doi.org/10.1038/s41598-020-60021-6
[2]  Abd-Elhamid, A. I., Emran, M., El-Sadek, M. H., El-Shanshory, A. A., Soliman, H. M., Akl, M. A., & Rashad, M. (2020). Enhanced Removal of Cationic Dye by Eco-Friendly Activated Biochar Derived from Rice Straw. Applied Water Science, 10, 45. https://doi.org/10.1007/s13201-019-1128-0
[3]  Sahu, S., Pahi, S., Sahu, J. K., Sahu, U. K., & Patel, R. K. (2020). Kendu (Diospyros Melanoxylon Roxb) Fruit Peel Activated Carbon - An Efficient Bioadsorbent for Methylene Blue Dye: Equilibrium, Kinetic, and Thermodynamic Study. Environmental Science and Pollution Research, 27, 22579-22592. https://doi.org/10.1007/s11356-020-08561-2
[4]  Wei, X., Wang, Y., Feng, Y., Xie, X., Li, X., & Yang, S. (2019). Different Adsorption-Degradation Behavior of Methylene Blue and Congo red in Nanoceria/H2O2 System under Alkaline Conditions. Scientific Reports, 9, 4964. https://doi.org/10.1038/s41598-018-36794-2
[5]  Derakhshan, Z., Baghapour, M. A., Ranjbar, M., & Faramarzian, M. (2013). Adsorption of Methylene Blue Dye from Aqueous Solutions by Modified Pumice Stone: Kinetics and Equilibrium Studies. Health Scope, 2(3), 136-144. https://doi.org/10.17795/jhealthscope-12492
[6]  Kosswattaarachchi, A. M., & Cook, T. R. (2018). Repurposing the Industrial Dye Methylene Blue as an Active Component for Redox Flow Batteries. ChemElectroChem, 5(22), 3437-3442. https://doi.org/10.1002/celc.201801097
[7]  Fernando, S. M., Tran, A., Soliman, K., Flynn, B., Oommen, T., Wenzhe, L., Adhikari, N. K. J., Kanji, S., Seely, A. J. E., Fox-Robichaud, A. E., Wax, R. S., Cook, D. J., Lamontagne, F., & Rochwerg, B. (2024). Methylene Blue in Septic Shock: A Systematic Review and Meta-Analysis. Critical Care Explorations, 6(7), e1110. https://doi.org/10.1097/CCE.0000000000001110
[8]  Bistas, E., & Sanghavi, D. K. (2023). Methylene Blue. In StatPearls [Internet]. StatPearls Publishing. https://www.ncbi.nlm.nih.gov/books/NBK557593/
[9]  Khan, I., Saeed, K., Zekker, I., Zhang, B., Hendi, A. H., Ahmad, A., Ahmad, S., Zada, N., Ahmad, H., Shah, L. A., Shah, T., & Khan, I. (2022). Review on Methylene Blue: Its Properties, Uses, Toxicity and Photodegradation. Water, 14(2), 242. https://doi.org/10.3390/w14020242
[10]   Liu, T., Li, Y., Du, Q., Sun, J., Jiao, Y., Yang, G., Wang, Z., Xia, Y., Zhang, W., Wang, K., Zhu, H. & Wu, D. (2012). Adsorption of Methylene Blue from Aqueous Solution by Graphene. Colloids and Surfaces B: Biointerfaces, 90, 197-203. https://doi.org/10.1016/j.colsurfb.2011.10.019
[11]   Imron, M. F., Kurniawan, S. B., Soegianto, A., & Wahyudianto, F. E. (2019). Phytoremediation of Methylene Blue Using Duckweed (Lemna minor). Heliyon, 5(8), e02206. https://doi.org/10.1016/j.heliyon.2019.e02206
[12]   Urucu, O. A., Garosi, B., & Musah, R. A. (2025). Efficient Phytoremediation of Methyl Red and Methylene Blue Dyes from Aqueous Solutions by Juncus effusus. ACS Omega, 10(2), 1943-1953. https://doi.org/10.1021/acsomega.4c07468
[13]   Sugha, A., & Bhatti, M. S. (2025). Optimization of Electrocoagulation Removal of a Mixture of Three Azo Dyes: Spectrophotometric Colour Characteristics for Best Operating Conditions. RSC Advances, 15(9), 6492-6505. https://doi.org/10.1039/D4RA08485C
[14]   Lau, Y. Y., Wong, Y. S., Teng, T. T., Morad, N., Rafatullah, M., & Ong, S. A. (2015). Degradation of Cationic and Anionic Dyes in Coagulation–Flocculation Process Using Bi-Functionalized Silica Hybrid with Aluminum-Ferric as Auxiliary Agent. RSC Advances, 5(43), 34206-34215. https://doi.org/10.1039/C5RA01346A
[15]   Cui, C., Li, D., & Wang, L. J. (2025). Biodegradable Genipin Cross‑Linked Chitosan/Pea Protein Isolate Sponges for Effective Adsorption of Methyl Blue: Batch Experiments and Quantum Chemical Analysis. Separation and Purification Technology, 358(part B), 130425. https://doi.org/10.1016/j.seppur.2024.130425
[16]   Abdelkader, M. S., Younis, S. A., El-Fawal, E. M., Ali, H. R., & Ibrahim, H. (2025). Ag3PO4@ZnO Kraft Lignin Composite for Optimized Photocatalytic Degradation of Methylene Blue Using Response Surface Methodology. Scientific Reports, 15, 20165. https://doi.org/10.1038/s41598-025-05597-7
[17]   Mahdavi, M., Mirmohammadi, M., Baghdadi, M., & Mahpishanian, S. (2022). Visible Light Photocatalytic Degradation and Pretreatment of Lignin Using Magnetic Graphitic Carbon Nitride for Enhancing Methane Production in Anaerobic Digestion. Fuel, 318, 123600. https://doi.org/10.1016/j.fuel.2022.123600
[18]   Hoang, N. T., Manh, T. D., Nguyen, V. T., Nga, N. T., Mwazighe, F. M., Nhi, B. D., Hoang, H. Y., Chang, S. W., Chung, W. J., & Nguyen, D. D. (2022). Kinetic Study on Methylene Blue Removal from Aqueous Solution Using UV/Chlorine Process and Its Combination with Other Advanced Oxidation Processes. Chemosphere, 308(part 3), 136457. https://doi.org/10.1016/j.chemosphere.2022.136457
[19]   Marey, A., Gado, W. S., Soliman, A. G., Masoud, A. M., El-Zahhar, A. A., Al-Hazmi, G. A., Taha, M. H., & El Naggar, A. M. (2024). Efficient Removal of Methylene Blue Dye from Wastewater Specimen Using Polystyrene Coated Nanoparticles of Silica. Inorganic Chemistry Communications, 160, 112018.
[20]   Hussein, E. B., & Rasheed, F. A. (2025). Innovative Use of Recycled Aluminum Adsorbent for Methylene Blue Adsorption and Post-Application for Soil Stabilization. Journal of Contaminant Hydrology, 272, 104553. https://doi.org/10.1016/j.jconhyd.2025.104553
[21]   Dimbo, D., Abewaa, M., Adino, E., Mengistu, A., Takele, T., Oro, A., & Rangaraju, M. (2024). Methylene Blue Adsorption from Aqueous Solution Using Activated Carbon of Spathodea campanulata. Results in Engineering, 21, 101910. https://doi.org/10.1016/j.rineng.2024.101910
[22]   Trivedi, Y., Sharma, M., Mishra, R. K., Sharma, A., Joshi, J., Gupta, A. B., Achintya, B., Shah, K., & Vuppaladadiyamd, A. K. (2025). Biochar Potential for Pollutant Removal During Wastewater Treatment: A Comprehensive Review of Separation Mechanisms, Technological Integration, and Process Analysis. Desalination, 600, 118509. https://doi.org/10.1016/j.desal.2024.118509
[23]   Le, T. P., Luong, H. V., Nguyen, H. N., Pham, T. K., Le, T. L., Tran, T. B., & Ngo, T. N. (2024). Insight into Adsorption-Desorption of Methylene Blue in Water Using Zeolite NaY: Kinetic, Isotherm and Thermodynamic Approaches. Results in Surfaces and Interfaces, 16, 100281. https://doi.org/10.1016/j.rsurfi.2024.100281
[24]   Li, S., Huang, L., Guo, W., Feng, X., Cao, Y., & Liao, B. (2024). Two‐Dimensional Copper‐Based Metal‐Organic Framework for Efficient Removal of Methylene Blue from Wastewater. European Journal of Inorganic Chemistry, 27(26), e202400240. https://doi.org/10.1002/ejic.202400240
[25]   Khan, M. A., ALOthman, Z. A., Naushad, M., Khan, M. R., & Luqman, M. (2015). Adsorption of Methylene Blue on Strongly Basic Anion Exchange Resin (Zerolit DMF): Kinetic, Isotherm, and Thermodynamic Studies. Desalination and Water Treatment, 53(2), 515-523. https://doi.org/10.1080/19443994.2013.838527
[26]   Farooq, N., Shanableh, A., Qureshi, A. M., Jabeen, S., & Rehman, A. (2022). Synthesis and Characterization of Clay Graphene Oxide Iron Oxide (Clay/GO/Fe2O3)-Nanocomposite for Adsorptive Removal of Methylene Blue Dye from Wastewater. Inorganic Chemistry Communications, 145, 109956. https://doi.org/10.1016/j.inoche.2022.109956
[27]   Turna, T., Solmaz, A., & Baran, A. (2025). Rapid Adsorption of Methylene Blue by Synthesizing Zinc Oxide Nanoparticles from Ocimum basilicum L. Waste. International Journal of Environmental Science and Technology, 22, 10049-10066. https://doi.org/10.1007/s13762-025-06492-4
[28]   Satyam, S., & Patra, S. (2024). Innovations and Challenges in Adsorption-Based Wastewater Remediation: A Comprehensive Review. Heliyon, 10(9), e29573. https://doi.org/10.1016/j.heliyon.2024.e29573
[29]   Fouda-Mbanga, B. G., Onotu, O. P., & Tywabi-Ngeva, Z. (2024). Advantages of the Reuse of Spent Adsorbents and Potential Applications in Environmental Remediation: A Review. Green Analytical Chemistry, 11, 100156. https://doi.org/10.1016/j.greeac.2024.100156
[30]   Akhtar, M. S., Ali, S., & Zaman, W. (2024). Innovative Adsorbents for Pollutant Removal: Exploring the Latest Research and Applications. Molecules, 29(18), 4317. https://doi.org/10.3390/molecules29184317
[31]   Wang, Y., Yang, P., Zheng, L., Shi, X., & Zheng, H. (2020). Carbon Nanomaterials with sp2 or/and sp Hybridization in Energy Conversion and Storage Applications: A Review. Energy Storage Materials, 26, 349-370. https://doi.org/10.1016/j.ensm.2019.11.006
[32]   Lim, S. Y., Shen, W., & Gao, Z. (2015). Carbon Quantum Dots and Their Applications. Chemical Society Reviews, 44(1), 362-381. https://doi.org/10.1039/C4CS00269E
[33]   Wu, M., Zhan, J., Geng, B., He, P., Wu, K., Wang, L., Xu, G., Li, Z., Yin, L., & Pan, D. (2017). Scalable Synthesis of Organic-Soluble Carbon Quantum Dots: Superior Optical Properties in Solvents, Solids, and LEDs. Nanoscale, 9(35), 13195-13202. https://doi.org/10.1039/C7NR04718E
[34]   Ukanwa, K. S., Patchigolla, K., Sakrabani, R., Anthony, E., & Mandavgane, S. (2019). A Review of Chemicals to Produce Activated Carbon from Agricultural Waste Biomass. Sustainability, 11(22), 6204. https://doi.org/10.3390/su11226204
[35]   Yavari, Z., & Noroozifar, M. (2017). Kinetic, Isotherm and Thermodynamic Studies with Linear and Non‑Linear Fitting for Cadmium(II) Removal by Black Carbon of Pine Cone. Water Science and Technology, 76(8), 2242-2253. https://doi.org/10.2166/wst.2017.375
[36]   Pundlik, R. C., Chowdhury, S. D., Dash, R. R., & Bhunia, P. (2021). Life-cycle assessment of agricultural waste-based and biomass-based adsorbents. In A. Pandey, R. Dayal Tyagi & S. Varjani (Eds), Biomass, Biofuels, Biochemicals (pp. 669-695). Elsevier Inc. https://doi.org/10.1016/B978-0-12-821878-5.00004-0
[37]   Akhtar, F., Andersson, L., Ogunwumi, S., Hedin, N., & Bergström, L. (2014). Structuring Adsorbents and Catalysts by Processing of Porous Powders. Journal of the European Ceramic Society, 34(7), 1643-1666. https://doi.org/10.1016/j.jeurceramsoc.2014.01.008
[38]   Baur, G. B., Yuranov, I., & Kiwi-Minsker, L. (2015). Activated Carbon Fibers Modified by Metal Oxide as Effective Structured Adsorbents for Acetaldehyde. Catalysis Today, 249, 252-258. https://doi.org/10.1016/j.cattod.2014.11.021
[39]   Peng, X., Luan, Z., Di, Z., Zhang, Z., & Zhu, C. (2005). Carbon Nanotubes-Iron Oxides Magnetic Composites as Adsorbent for Removal of Pb (II) and Cu (II) from Water. Carbon, 43(4), 880-883. https://doi.org/10.1016/j.carbon.2004.11.009
[40]   Hu, J., Song, Z., Chen, L., Yang, H., Li, J., & Richards, R. (2010). Adsorption Properties of MgO(111) Nanoplates for the Dye Pollutants from Wastewater. Journal of Chemical & Engineering Data, 55(9), 3742-3748. https://doi.org/10.1021/je100274e
[41]   Khan, M. M., Khan, W., Ahamed, M., & Alhazaa, A. N. (2017). Microstructural Properties and Enhanced Photocatalytic Performance of Zn Doped CeO2 Nanocrystals. Scientific Reports, 7, 12560. https://doi.org/10.1038/s41598-017-11074-7
[42]   Hassanzadeh-Tabrizi, S. A., Motlagh, M. M., & Salahshour, S. (2016). Synthesis of ZnO/CuO Nanocomposite Immobilized on γ-Al2O3 and Application for Removal of Methyl Orange. Applied Surface Science, 384, 237-243. https://doi.org/10.1016/j.apsusc.2016.04.165
[43]   Koohestanian, E., Samimi, A., Mohebbi-Kalhori, D., & Sadeghi, J. (2017). Sensitivity Analysis and Multi-Objective Optimization of CO2CPU Process Using Response Surface Methodology. Energy, 122, 570-578. https://doi.org/10.1016/j.energy.2017.01.129
[44]   Mehta, A., Mishra, A., Basu, S., Shetti, N. P., Reddy, K. R., Saleh, T. A., & Aminabhavi, T. M. (2019). Band Gap Tuning and Surface Modification of Carbon Dots for Sustainable Environmental Remediation and Photocatalytic Hydrogen Production - A Review. Journal of Environmental Management, 250, 109486. https://doi.org/10.1016/j.jenvman.2019.109486
[45]   Gomroki, S., Yavari, Z., Abbasian, A. R., Afarani, M. S., & Noroozifar, M. (2022). Stabilizing Nano‑Pd on Porous Li2TiO3 via Chemical and Electrochemical Reduction Systems for the Electrooxidation of Ethylene Glycol. Materials Chemistry and Physics, 281, 125896. https://doi.org/10.1016/j.matchemphys.2022.125896
[46]   Hosseini, S. A., Abbasian, A. R., Gholipoor, O., Ranjan, S., & Dasgupta, N. (2019). Adsorptive Removal of Arsenic from Real Sample of Polluted Water Using Magnetic GO/ZnFe2O4 Nanocomposite and ZnFe2O4 Nanospinel. International Journal of Environmental Science and Technology, 16, 7455-7466. https://doi.org/10.1007/s13762-018-2140-x
[47]   Nakamoto, K. (2008). Infrared and Raman Spectra of Inorganic and Coordination Compounds, Part B: Applications in Coordination, Organometallic, and Bioinorganic Chemistry. John Wiley & Sons. https://doi.org/10.1002/9780470405888
[48]   Mahalingam, T., Selvakumar, C., Kumar, E. R., & Venkatachalam, T. (2017). Structural, Optical, Morphological and Thermal Properties of TiO2-Al and TiO2-Al2O3 Composite Powders by Ball Milling. Physics Letters A, 381(21), 1815-1819. https://doi.org/10.1016/j.physleta.2017.02.053
[49]   Emam, A. N., Loutfy, S. A., Mostafa, A. A., Awad, H., & Mohamed, M. B. (2017). Cyto-Toxicity, Biocompatibility and Cellular Response of Carbon Dots–Plasmonic Based Nano-Hybrids for Bioimaging. RSC Advances, 7(38), 23502-23514. https://doi.org/10.1039/C7RA01423F
[50]   Gao, Y., Li, Y., Zhang, L., Huang, H., Hu, J., Shah, S. M., & Su, X. (2012). Adsorption and Removal of Tetracycline Antibiotics from Aqueous Solution by Graphene Oxide. Journal of Colloid and Interface Science, 368(1), 540-546. https://doi.org/10.1016/j.jcis.2011.11.015
[51]   Chao, Y., Zhu, W., Wu, X., Hou, F., Xun, S., Wu, P., Ji, H., Xu, H., & Li, H. (2014). Application of Graphene-Like Layered Molybdenum Disulfide and Its Excellent Adsorption Behavior for Doxycycline Antibiotic. Chemical Engineering Journal, 243, 60-67. https://doi.org/10.1016/j.cej.2013.12.048
[52]   Foo, K. Y., & Hameed, B. H. (2010). Insights into the Modeling of Adsorption Isotherm Systems. Chemical Engineering Journal, 156(1), 2-10. https://doi.org/10.1016/j.cej.2009.09.013
[53]   Akhtar, M., Sarfraz, M., Ahmad, M., Raza, N., & Zhang, L. (2025). Use of Low‑Cost Adsorbent for Waste Water Treatment: Recent Progress, New Trend and Future Perspectives. Desalination and Water Treatment, 321, 100914. https://doi.org/10.1016/j.dwt.2024.100914
[54]   López-Luna, J., Ramírez-Montes, L. E., Martinez-Vargas, S., Martínez, A. I., Mijangos-Ricardez, O. F., González-Chávez, M. D., Carrillo-González, R., Solís-Domínguez, F. A., Cuevas-Díaz, M. D., & Vázquez-Hipólito, V. (2019). Linear and Nonlinear Kinetic and Isotherm Adsorption Models for Arsenic Removal by Manganese Ferrite Nanoparticles. SN Applied Sciences, 1(8), 950. https://doi.org/10.1007/s42452-019-0977-3
[55]   Mercado-Borrayo, B. M., Schouwenaars, R., Litter, M. I., Montoya-Bautista, C. V., & Ramírez-Zamora, R. M. (2014). Metallurgical slag as an efficient and economical adsorbent of arsenic. In S. Ahuja (Ed.), Water Reclamation and Sustainability (pp. 95-114). Elsevier. https://doi.org/10.1016/B978-0-12-411645-0.00005-5
[56]   Batzias, F. A., & Sidiras, D. K. (2004). Dye Adsorption by Calcium Chloride Treated Beech Sawdust in Batch and Fixed-Bed Systems. Journal of Hazardous Materials, 114(1-3), 167-174. https://doi.org/10.1016/j.jhazmat.2004.08.014
[57]   Khattri, S. D., & Singh, M. K. (2000). Colour Removal from Synthetic Dye Wastewater Using a Bioadsorbent. Water, Air, and Soil Pollution, 120(3), 283-294. https://doi.org/10.1023/A:1005207803041
[58]   Tsai, W. T., Hsu, H. C., Su, T. Y., Lin, K. Y., & Lin, C. M. (2008). Removal of Basic Dye (Methylene Blue) from Wastewaters Utilizing Beer Brewery Waste. Journal of Hazardous Materials, 154(1-3), 73-78. https://doi.org/10.1016/j.jhazmat.2007.09.107
[59]   Ozdemir, F. A., Demirata, B., & Apak, R. (2009). Adsorptive Removal of Methylene Blue from Simulated Dyeing Wastewater with Melamine‐Formaldehyde‐Urea Resin. Journal of Applied Polymer Science, 112(6), 3442-3448. https://doi.org/10.1002/app.29835
[60]   Kavitha, D., & Namasivayam, C. (2007). Experimental and Kinetic Studies on Methylene Blue Adsorption by Coir Pith Carbon. Bioresource Technology, 98(1), 14-21. https://doi.org/10.1016/j.biortech.2005.12.008
[61]   Srihari, V., & Das, A. (2008). The Kinetic and Thermodynamic Studies of Phenol-Sorption onto Three Agro-Based Carbons. Desalination, 225(1-3), 220-234. https://doi.org/10.1016/j.desal.2007.07.008
[62]   Jamal, R., Zhang, L., Wang, M., Zhao, Q., & Abdiryim, T. (2016). Synthesis of Poly(3,4-propylenedioxy-thiophene)/MnO2 Composites and Their Applications in the Adsorptive Removal of Methylene Blue. Progress in Natural Science: Materials International, 26(1), 32-40. https://doi.org/10.1016/j.pnsc.2016.01.001
[63]   Peighambardoust, S. J., Rezaei-Aghdam, S., Niroumand, J. S., Pakdel, P. M., & Sillanpää, M. (2025). Efficient Methylene Blue Elimination from Water Media by Nanocomposite Adsorbent-Based Carboxymethyl Cellulose-Grafted Poly(acrylamide)/ Magnetic Biochar Decorated with ZIF-67. RSC Advances, 15(39), 32407-32423. https://doi.org/10.1039/D5RA03796D
Volume 11, Issue 2
December 2025
Pages 101-116

  • Receive Date 09 December 2025
  • Revise Date 30 March 2026
  • Accept Date 31 March 2026