Abstract
This study presents a sustainable approach for Methylene Blue (MB) dye removal using pristine, non-activated biochar derived from orange peel waste via Microwave-Assisted Pyrolysis (MAP). The key novelty lies in the systematic comparison of the biochar’s adsorption performance under both pH-controlled (constant pH 4) and unregulated pH conditions, demonstrating that pH regulation is essential for optimizing adsorption efficiency. The resulting biochar exhibited a high fixed carbon content (60.89%), an alkaline surface (Point of zero charge (pHpzc) = 11.20, ZPotential = 0.1 mV @ pH 9), and oxygenated functional groups. Best MB removal of 83% was achieved at pH 4, despite the expected electrostatic repulsion. Kinetic studies showed the best fit with the Elovich model, indicating a heterogeneous surface. The Langmuir isotherm accurately described the equilibrium data, revealing a maximum adsorption capacity (qmax) of 20.57 mg g⁻1 under pH-controlled conditions, representing an 83% increase over the 11.24 mg g⁻1 obtained in the unregulated scenario. Thermodynamic analysis confirmed the process is spontaneous (ΔG° < 0), endothermic (ΔH° = + 4.88 kJ mol⁻1 at constant pH), and governed by physisorption mechanisms, including hydrogen bonding and π-π interactions. This work demonstrates that pristine orange peel biochar generated via MAP is a highly effective adsorbent and highlights the critical impact of pH control on improving adsorption capacity and elucidating the dominant physisorption mechanisms.
Data availability
The datasets used and/or analyzed during the current study are available from the corresponding author on reasonable request.
References
Lin, J. et al. Environmental impacts and remediation of dye-containing wastewater. Nat. Rev. Earth Environ. 4, 785–803 (2023).
Dutta, S. et al. Contamination of textile dyes in aquatic environment: Adverse impacts on aquatic ecosystem and human health, and its management using bioremediation. J. Environ. Manage. 353, 120103 (2024).
Kobylewski, S. & Jacobson, M. F. Toxicology of food dyes. Int. J. Occup. Environ. Health 18, 220–246 (2012).
Khan, I. et al. Review on methylene blue: its properties, uses, toxicity and photodegradation. Water 14, 242 (2022).
Kurniasih, M., Aprilita, N. H., Roto, R. & Mudasir, M. Modification of coal fly ash for high capacity adsorption of methylene blue. Case Stud. Chem. Environ. Eng. 11, 101101 (2025).
Al-Tohamy, R. et al. A critical review on the treatment of dye-containing wastewater: Ecotoxicological and health concerns of textile dyes and possible remediation approaches for environmental safety. Ecotoxicol. Environ. Saf. 231, 113160 (2022).
León, M., Silva, J., Carrasco, S. & Barrientos, N. Design, cost estimation and sensitivity analysis for a production process of activated carbon from waste nutshells by physical activation. Processes 8, 945 (2020).
Jagadeesh, N. & Sundaram, B. Adsorption of pollutants from wastewater by biochar: a review. J. Hazard. Mater. Adv. 9, 100226 (2023).
Michael-Igolima, U., Abbey, S. J., Ifelebuegu, A. O. & Eyo, E. U. Modified orange peel waste as a sustainable material for adsorption of contaminants. Materials 16, 1092 (2023).
Ayala, J. R. et al. Characterization of orange peel waste and valorization to obtain reducing sugars. Molecules 26, 1348 (2021).
Chen, Z. et al. Enhanced adsorption of phosphate on orange peel-based biochar activated by Ca/Zn composite: Adsorption efficiency and mechanisms. Colloids Surf. Physicochem. Eng. Asp. 651, 129728 (2022).
Afolabi, F. O. & Musonge, P. Synthesis, characterization, and biosorption of Cu2+ and Pb2+ ions from an aqueous solution using biochar derived from orange peels. Molecules 28, 7050 (2023).
Potnuri, R. et al. A review on analysis of biochar produced from microwave-assisted pyrolysis of agricultural waste biomass. J. Anal. Appl. Pyrolysis 173, 106094 (2023).
Shirvanimoghaddam, K. et al. Microwave synthesis of biochar for environmental applications. J. Anal. Appl. Pyrolysis 161, 105415 (2022).
Zhang, Y., Fan, S., Liu, T., Fu, W. & Li, B. A review of biochar prepared by microwave-assisted pyrolysis of organic wastes. Sustain. Energy Technol. Assess. 50, 101873 (2022).
Ethaib, S., Omar, R., Kamal, S. M. M., Awang Biak, D. R. & Zubaidi, S. L. Microwave-assisted pyrolysis of biomass waste: a mini review. Processes 8, 1190 (2020).
Lam, S. S. et al. Activated carbon for catalyst support from microwave pyrolysis of orange peel. Waste Biomass Valorization 8, 2109–2119 (2017).
Jawad, A. H., Hapiz, A. & Wu, R. Mixed fruit Citrullus lanatus and Citrus sinensis wastes for mesoporous activated carbon via microwave assisted H3PO4 activation: Optimization for methylene blue dye removal. Biomass Convers. Biorefinery 15, 6989–7003 (2025).
Correa-Abril, J. et al. Adsorption dynamics of Cd2+(aq) on microwave-synthetized pristine biochar from cocoa pod husk: Green, experimental, and DFT approaches. iScience 27, 109958 (2024).
Zambrano-Intriago, L. et al. Kinetics, equilibrium, and thermodynamics of the blue 19 dye adsorption process using residual biomass attained from rice cultivation. Biomass Convers. Biorefinery 12, 3843–3855 (2022).
Andrade, C. et al. Adsorption behavior and mechanism of oxytetracycline on rice husk ash: kinetics, equilibrium, and thermodynamics of the process. Water. Air. Soil Pollut. 231, 103 (2020).
Jayakumar, M. et al. Comprehensive review on lignocellulosic biomass derived biochar production, characterization, utilization and applications. Chemosphere 345, 140515 (2023).
Mirkarimi, S. M. R., Bensaid, S., Negro, V. & Chiaramonti, D. Review of methane cracking over carbon-based catalyst for energy and fuels. Renew. Sustain. Energy Rev. 187, 113747 (2023).
You, X., Wang, R., Zhu, Y., Sui, W. & Cheng, D. Comparison of adsorption properties of a cellulose-rich modified rice husk for the removal of methylene blue and aluminum (III) from their aqueous solution. Ind. Crops Prod. 170, 113687 (2021).
García, D. B., Sanchez, M. C., Bacigalupe, A., Escobar, M. M. & Mansilla, M. A. Chapter 14 - Green rubber composites. In Green Sustainable Process for Chemical and Environmental Engineering and Science (ed. Altalhi, T.) 273–312 (Elsevier, 2022). https://doi.org/10.1016/B978-0-323-99643-3.00008-5.
Al-Janabi, E. S. H. & Yasen, S. S. Determination of chemical composition and antioxidants of wheat flour, orange peel powder and manufactured biscuits. AIP Conf. Proc. 2839, 060006 (2023).
Li, S. & Tasnady, D. Biochar for soil carbon sequestration: current knowledge, mechanisms, and future perspectives. C 9, 67 (2023).
Duan, C. et al. A review on nitrogen transformation mechanism during biomass pyrolysis. J. Anal. Appl. Pyrolysis 184, 106863 (2024).
Liu, H. et al. Emission control of NOx precursors during sewage sludge pyrolysis using an integrated pretreatment of Fenton peroxidation and CaO conditioning. Fuel 195, 208–216 (2017).
Bakshi, S., Banik, C. & Laird, D. A. Estimating the organic oxygen content of biochar. Sci. Rep. 10, 13082 (2020).
Mastalerz, M., Drobniak, A., Liu, B. & Sauer, P. E. Reflectance as an indicator of biochar permanence. Int. J. Coal Geol. 306, 104809 (2025).
Chen, Y., Zhang, X., Chen, W., Yang, H. & Chen, H. The structure evolution of biochar from biomass pyrolysis and its correlation with gas pollutant adsorption performance. Bioresour. Technol. 246, 101–109 (2017).
Nuryana, D. et al. Methylene blue removal using coconut shell biochar synthesized through microwave-assisted pyrolysis. J. Teknol. Sci. Eng. https://doi.org/10.11113/jt.v82.14359 (2020).
Xia, Y., Yao, Q., Zhang, W., Zhang, Y. & Zhao, M. Comparative adsorption of methylene blue by magnetic baker’s yeast and EDTAD-modified magnetic baker’s yeast: Equilibrium and kinetic study. Arab. J. Chem. 12, 2448–2456 (2015).
Afolabi, F. O., Musonge, P. & Bakare, B. F. Adsorption of copper and lead ions in a binary system onto orange peels: optimization, equilibrium, and kinetic study. Sustainability 14, 10860 (2022).
Premalatha, R. P. et al. A review on biochar’s effect on soil properties and crop growth. Front. Energy Res. 11, 1092637 (2023).
Geleto, M. A. et al. Influence of pyrolysis temperature and feedstock biomass on Cu2+, Pb2+, and Zn2+ sorption capacity of biochar. Int. J. Environ. Sci. Technol. 19, 11857–11866 (2022).
Albalasmeh, A. et al. Characterization and Artificial Neural Networks Modelling of methylene blue adsorption of biochar derived from agricultural residues: Effect of biomass type, pyrolysis temperature, particle size. J. Saudi Chem. Soc. 24, 811–823 (2020).
Breen, R., Goggin, C., Holmes, J. D. & Collins, G. A collaborative cocurricular undergraduate research experience on sustainable materials: analysis of biochar using the Boehm titration and spectroscopic techniques. J. Chem. Educ. 102, 1323–1332 (2025).
Amalina, F., Razak, A. S. A., Krishnan, S., Zularisam, A. W. & Nasrullah, M. A comprehensive assessment of the method for producing biochar, its characterization, stability, and potential applications in regenerative economic sustainability – A review. Clean. Mater. 3, 100045 (2022).
Barszcz, W., Łożyńska, M. & Molenda, J. Impact of pyrolysis process conditions on the structure of biochar obtained from apple waste. Sci. Rep. 14, 10501 (2024).
Lam, S. S. et al. Microwave-assisted pyrolysis with chemical activation, an innovative method to convert orange peel into activated carbon with improved properties as dye adsorbent. J. Clean. Prod. 162, 1376–1387 (2017).
Ho, Y. S. & McKay, G. Pseudo-second order model for sorption processes. Process Biochem. 34, 451–465 (1999).
Ahmaruzzaman, M. & Gupta, V. K. Rice husk and its ash as low-cost adsorbents in water and wastewater treatment. Ind. Eng. Chem. Res. 50, 13589–13613 (2011).
Dotto, J., Fagundes-Klen, M. R., Veit, M. T., Palácio, S. M. & Bergamasco, R. Performance of different coagulants in the coagulation/flocculation process of textile wastewater. J. Clean. Prod. 208, 656–665 (2019).
Sukor, N. F. & Jusoh, R. Hybrid activated carbon/ maltodextrin-functionalized fibrous silica for acetaminophen and amoxicillin adsorption: Advanced statistical physics modelling. Environ. Res. 278, 121691 (2025).
Al-Harby, N. F., Albahly, E. F. & Mohamed, N. A. Kinetics, isotherm and thermodynamic studies for efficient adsorption of Congo red dye from aqueous solution onto novel Cyanoguanidine-modified chitosan adsorbent. Polymers 13, 4446 (2021).
Liu, B. et al. Temperature-induced adsorption and desorption of phosphate on poly(acrylic acid-co-N-[3-(dimethylamino)propyl]acrylamide) hydrogels in aqueous solutions. Desalination Water Treat. 160, 260–267 (2019).
Kumar, M. & Tamilarasan, R. Kinetics, equilibrium data and modeling studies for the sorption of chromium by Prosopis juliflora bark carbon. Arab. J. Chem. 10, S1567–S1577 (2013).
Ao, C. et al. Impact of external conditions on the desorption and degradation capacity of biochar for rhodamine B. Molecules 30, 1717 (2025).
Maaoui, A. et al. Calcium-rich biochar derived from cactus feedstock and its efficient adsorption properties for industrial dye. Appl. Sci. 15, 894 (2025).
Saha, N. et al. Cationic dye adsorption on hydrochars of winery and citrus juice industries residues: performance, mechanism, and thermodynamics. Energies 13, 4686 (2020).
Tenea, A.-G. et al. Exploring adsorption dynamics of heavy metals onto varied commercial microplastic substrates: Isothermal models and kinetics analysis. Heliyon 10, e35364 (2024).
Ren, Y., Geng, W., Xu, R., Wang, P. & Zhao, H. Tuning electronic and pore structures of biochar via nitrogen and magnesium doping for superior methylene blue adsorption: synergistic mechanisms and kinetic analysis. ACS Omega 10, 31679–31692 (2025).
Chu, K. H. et al. The Redlich-Peterson isotherm for aqueous phase adsorption: Pitfalls in data analysis and interpretation. Chem. Eng. Sci. 285, 119573 (2024).
Hanafi, N. A. M. et al. Optimized removal process and tailored adsorption mechanism of crystal violet and methylene blue dyes by activated carbon derived from mixed orange peel and watermelon rind using microwave-induced ZnCl2 activation. Biomass Convers. Biorefinery 14, 28415–28427 (2024).
Amin, M. T., Alazba, A. A. & Shafiq, M. Comparative study for adsorption of methylene blue dye on biochar derived from orange peel and banana biomass in aqueous solutions. Environ. Monit. Assess. 191, 735 (2019).
Gunay Gurer, A., Aktas, K., Ozkaleli Akcetin, M., Erdem Unsar, A. & Asilturk, M. Adsorption isotherms, thermodynamics, and kinetic modeling of methylene blue onto novel carbonaceous adsorbent derived from bitter orange peels. Water. Air. Soil Pollut. 232, 138 (2021).
Ding, W. et al. Environmental applications of lignin-based hydrogels for Cu remediation in water and soil: adsorption mechanisms and passivation effects. Environ. Res. 250, 118442 (2024).
Zaheer, Z., AbuBaker Bawazir, W., Al-Bukhari, S. M. & Basaleh, A. S. Adsorption, equilibrium isotherm, and thermodynamic studies to the removal of acid orange 7. Mater. Chem. Phys. 232, 109–120 (2019).
Huang, Y.-T. & Shih, M.-C. Kinetic, isotherm, and thermodynamic modeling of methylene blue adsorption using natural rice husk: a sustainable approach. Separations 12, 189 (2025).
Garcia, E. M., Taroco, H. A. & Melo, J. O. F. Highly efficient Eugenia dysenterica DC seeds biomass as adsorbent for methylene blue removal. Discov. Chem. 2, 11 (2025).
El-Rayyes, A. et al. Thermodynamic, isotherm and kinetic studies lead ions adsorption onto Manihot esculenta chaff surface. Sci. Rep. 15, 27672 (2025).
Salgın, U., Alomari, İ, Soyer, N. & Salgın, S. Adsorption of bisphenol A onto β-cyclodextrin–based nanosponges and innovative supercritical green regeneration of the sustainable adsorbent. Polymers 17, 856 (2025).
Xiang, L. et al. Potential hazards of biochar: The negative environmental impacts of biochar applications. J. Hazard. Mater. 420, 126611 (2021).
Acknowledgements
The authors would like to express their gratitude to all the individuals and institutional collaborators who have provided their support and assistance and to the Universidad Central del Ecuador for financing the Senior Project DI-CONV-2022-025 and DI-CONV-2023-029. We are also very grateful to Dr. Carsten Natzeck from the Institute of Functional Interfaces – Karlsruhe Institute of Technology for his valuable support on SEM images and EDX analysis, the laboratory of research activities (LISE) of the Faculty of Chemical Engineering, as well as to Dr. Pablo Bonilla of the laboratory of nanomaterials of the Faculty of Chemistry for his support on ZP measurements.
Funding
This work was financed by the Universidad Central del Ecuador and it´s Dirección de Investigación via the Senior Project “Desarrollo de un adsorbente basado en biocarbón de Theobroma cacao y marco metal orgánico (MOF) para la remoción de fármacos en aguas residuales sintéticas” (No. DI-CONV-2023-029).
Author information
Authors and Affiliations
Contributions
Ullrich Stahl: Writing—review & editing, Writing—original draft, Methodology, Investigation, Formal analysis. Elvia V. Cabrera and Jhonny Correa-Abril: Writing—review & editing, Validation, Supervision, Formal analysis, Conceptualization. Nilo Robles: Writing, Validation, Supervision, Formal analysis, J. L. López Terán: Project administration, Funding acquisition.
Corresponding author
Ethics declarations
Competing interests
The authors declare no competing interests.
Additional information
Publisher’s note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary Information
Rights and permissions
Open Access This article is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License, which permits any non-commercial use, sharing, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if you modified the licensed material. You do not have permission under this licence to share adapted material derived from this article or parts of it. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by-nc-nd/4.0/.
About this article
Cite this article
Correa-Abril, J., Cabrera, E.V., Robles, N. et al. Kinetic, equilibrium, and thermodynamic study of Methylene Blue adsorption on orange peel biochar prepared by microwave-assisted pyrolysis. Sci Rep (2026). https://doi.org/10.1038/s41598-026-36741-6
Received:
Accepted:
Published:
DOI: https://doi.org/10.1038/s41598-026-36741-6