Dopamine-mediated Green Synthesis of Halloysite Nanotube-functionalized Jute Fiber Geopolymer Composites for CO₂ Capture and Mineral Immobilization
J. Environ. Nanotechnol., Volume 15, No 3 (September 2026) pp. 882-909
Abstract
The increasing level of atmospheric CO₂ and the need for long-term carbon storage have created a demand for construction materials that can combine structural performance with carbon management. Conventional geopolymer materials mainly focus on mechanical strength and durability, while their potential for simultaneous CO₂ capture and permanent mineral storage remains less explored. This study develops a multifunctional geopolymer composite integrating metakaolin-GGBFS binder with jute fibers and dopamine-functionalized halloysite nanotubes (D-HNTs) for simultaneous structural reinforcement and CO₂ capture. D-HNTs were prepared via aqueous dopamine functionalization and incorporated at 1.5-3.0 wt%. The optimized GP-JF-DHNTs-S2 composite achieved a 28-day compressive strength of 31.2 MPa and a flexural strength of 5.7 MPa, with impact resistance enhanced by 68% over the control. CO₂ uptake reached 1.03 mmol/g at 25 °C and 1 atm, a 3.4-fold improvement over control geopolymer. Over 80% of equilibrium uptake occurred within 30 minutes. XRD, FTIR, and XPS analyses confirmed carbonate formation, with 7.0 wt% CaCO₃ precipitated. The material retained 85% of initial CO₂ adsorption capacity after 10 cycles, demonstrating permanent mineral immobilization. This hierarchical composite provides a dual-functional platform for carbon-storing construction materials.
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Reference
Abdullayev, E. and Lvov, Y., Halloysite for controllable loading and release, Develop. Clay Sci., 7, 554-605 (2016).
https://doi.org/10.1016/B978-0-08-100293-3.00022-4
Ahmed, J. P. S., Kaviyan, M., Sivakumar, Y. and Shanmugavel, S., Exploring the role of halloysite nanotubes in improving carbon fiber reinforced composite performance across diverse temperatures, Eng. Res. Exp., 7(4), 045521 (2025).
https://doi.org/10.1088/2631-8695/ae0f04
Al-Naghi, A. A., Ghazouani, N. and Elhadi, K. M., Thermo-Carbonation synergy for enhanced CO₂ sequestration and performance of activated bauxite residue-based geopolymer composites, J. Sustain. Cem. Based Mater., 1-23 (2026).
https://doi.org/10.1080/21650373.2026.2696353
Andrew, R. M., Global CO₂ emissions from cement production, 1928–2018, Earth Syst. Sci. Data, 11(4), 1675-1710 (2019).
https://doi.org/10.5194/essd-11-1675-2019
Bakri, O. M. and Mahmoud, A. A., CO₂-Binder Reaction Mechanisms in Geopolymer Wellbore Cements: Alternatives to API Class G Cement in CO₂-Rich Environments (CCS), Mol., 31(4), 620 (2026).
https://doi.org/10.3390/molecules31040620
Bernal, S. A., Microstructural changes induced by CO₂ exposure in alkali-activated slag/metakaolin pastes, Front. Mater., 3, 43 (2016).
https://doi.org/10.3389/fmats.2016.00043
Çevik, A. and Niş, A., Introduction to fiber-reinforced alkali-activated composites, Adv. Fib. Reinforce. Alkali-Activated Compos., 1-21 (2023).
https://doi.org/10.1016/B978-0-443-15301-3.00007-5
Chaggar, P. K., Javan, K., Duarte, M. C., Darestani, M. and Markhali, B. P., Dynamic CO₂ sequestration: from global emission challenges to sustainable capture through geopolymer technologies, Environ. Sci. Pollut. Res., 32(46), 26068-26087 (2025).
https://doi.org/10.1007/s11356-025-37222-5
Chen, H., Yang, Y., Wei, W., Cavallaro, G., Zhai, Z., Zhao, Y., Wang, D., Chen, S., Shang, H. and Zhang, B., Superhydrophobic halloysite-based porous foamed geopolymer for efficient phase change material encapsulation with enhanced thermal management performance, Appl. Clay Sci., 284, 108133 (2026).
https://doi.org/10.1016/j.clay.2026.108133
Chen, Q., Chen, Y., Kang, J. and Chen, F., Carbonation impact on the stabilization of heavy metals in carbon-rich geopolymers based on gasification slag and fly ash, Environ. Pollut., 382, 126671 (2025).
https://doi.org/10.1016/j.envpol.2025.126671
da Rocha Loures, F. S., Sichonany, A. V., Mortari, S. R., Floss, M. F., da Silva, W. L. and da Silva, C. L., Aplicação de nanotubos de carbono em concreto: uma revisão técnica, Disciplinarum Scientia Naturais e Tecnológicas, 27(2), 61-85 (2026).
https://doi.org/10.37779/nt.v27i2.5615
Das, S. C., Das, S. C., Rahman, M. M., Sayeed, M. A., Khan, M. M., Jahan, M. S. and Islam, T., Analysis of mechanical and thermal properties of hybrid FRP composites with short jute, coir and glass fibers—effects of different fiber loading and waste valorization, Mater. Circ. Econ., 7(1), 42 (2025).
https://doi.org/10.1007/s42824-025-00197-2
Davidovits, J., Geopolymers based on natural and synthetic metakaolin: a critical review, Proce. 41st Int. Conf. Adv. Ceram. Compos. Ceram. Eng. Sci. Proce., 38(3), 38 (2018).
https://doi.org/10.1002/9781119474746.ch19
Fan, L., Xu, F., Wang, S., Yu, Y., Li, P., Zhang, J. and Yu, L., Role of halloysite nanotubes in modulating the mechanical and microstructural characteristics of geopolymer concrete under thermal curing, Constr. Build. Mater., 472, 140897 (2025).
https://doi.org/10.1016/j.conbuildmat.2025.140897
Feng, J., Fan, H., Zha, D. A., Wang, L. and Jin, Z., Characterizations of the formation of polydopamine-coated halloysite nanotubes in various pH environments, Langmuir, 32(40), 10377-10386 (2016).
https://doi.org/10.1021/acs.langmuir.6b02948
Hassan, H. S., Shi, C., Hashem, F. S., El-Magd, S. A., Maged, A., Abdel-Gawwad, H. A. and Pfeiffer, H., Industrial waste recycling approach: An ecofriendly geopolymer binder for clean and sustainable environments (A 24-h green recycling process), J. Environ. Manage., 377, 124568 (2025).
https://doi.org/10.1016/j.jenvman.2025.124568
Islam, S., Karim, F. E. and Islam, M. R., Assessing the consequences of water retention on the structural integrity of jute fiber and its composites: a review, SPE Polym., 5(4), 457-480 (2024).
https://doi.org/10.1002/pls2.10142
Jagajeevan, V. and Sivakumar, V. L., Environmental fate mapping of lead-free piezoelectrics: Synergistic stress-induced leaching kinetics and multi-trophic dose-response in BFO/rGO hybrids, Chemosphere, 409, 145001 (2026).
https://doi.org/10.1016/j.chemosphere.2026.145001
Joussein, E., Petit, S., Churchman, J., Theng, B., Righi, D. and Delvaux, B. J., Halloysite clay minerals—a review, Clay Miner., 40(4), 383-426 (2005).
https://doi.org/10.1180/0009855054040180
Kavitha, S. S., Sarker, P. K., Madhavan, M. K. and Jayanarayanan, K., Sustainable approach for the confinement of concrete cylinders using fiber-reinforced polymers with bio-based hemp and halloysite nano tubes, Polym. Compos., 47(12), 11377-11393 (2026).
https://doi.org/10.1002/pc.71028
Li, B., Ma, J., Long, K., Zhang, J., Gao, Y. and Liu, H., CO₂ mineralization with fly ash for underground carbon-negative backfill: Carbon sequestration and heavy metal immobilization, J. CO₂ Util., 106, 103366 (2026a).
https://doi.org/10.1016/j.jcou.2026.103366
Li, H., Gao, L., Huang, L. and Li, Y., A comprehensive environmental impact evaluation of underground wastewater treatment plant: Integrating greenhouse gas emissions, environment footprint, and economic assessments, Process Saf. Environ. Prot., 211, 108748 (2026b).
https://doi.org/10.1016/j.psep.2026.108748
Lo Bianco, A., Calvino, M. M., Cavallaro, G., Lisuzzo, L., Pasbakhsh, P., Milioto, S., Lazzara, G. and Lvov, Y., Flame-resistant inorganic films by self-assembly of clay nanotubes and their conversion to geopolymer for CO₂ capture, Small, 20(51), 2406812 (2024).
https://doi.org/10.1002/smll.202406812
Mastali, M., Kinnunen, P., Isomoisio, H., Karhu, M. and Illikainen, M., Mechanical and acoustic properties of fiber-reinforced alkali-activated slag foam concretes containing lightweight structural aggregates, Constr. Build. Mater., 187, 371-381 (2018).
https://doi.org/10.1016/j.conbuildmat.2018.07.228
Murmu, A. L., Dhole, N. and Patel, A., Stabilisation of black cotton soil for subgrade application using fly ash geopolymer, Road Mater. Pavement Des., 21(3), 867-885 (2020).
https://doi.org/10.1080/14680629.2018.1530131
Nanthini, M., Ganesan, R. and Jaganathan, V., Incorporation of nanoalumina in potassium feldspar-based phosphoric acid activated geopolymer composites: a sustainable approach, J. Environ. Nanotechnol., 13(3), 89-98 (2024a).
https://doi.org/10.13074/jent.2024.09.243840
Pan, Z., Zhang, C., Li, Y. and Yang, C., Solidification/stabilization of gold ore tailings powder using sustainable waste-based composite geopolymer, Eng. Geol., 309, 106793 (2022).
https://doi.org/10.1016/j.enggeo.2022.106793
Praveenkumar, S., Vishvanathperumal, S., Ramu, K. N. and Manimaran, K., Influence of halloysite nanotubes (HNTs) and their TESPT-, APTES-, and GPTMS-modified forms on the curing, mechanical, and swelling behavior of SBR/NBR composites, J. Mater. Eng. Perform., 35, 27157-27172 (2026).
https://doi.org/10.1007/s11665-026-13530-w
Provis, J. L., Palomo, A. and Shi, C., Advances in understanding alkali-activated materials, Cem. Concr. Res., 78, 110-125 (2015).
https://doi.org/10.1016/j.cemconres.2015.04.013
Reddy, A. S., Iyer, K. K., Rotte, V. M. and Dave, T. N., Performance of alkali activated slag stabilized landfill mined soil-like fraction exposed to different climatic conditions, Int. J. Geosynth. Ground Eng., 10(5), 80 (2024).
https://doi.org/10.1007/s40891-024-00593-9
Shi, J., Shen, Y., Zhang, W., Fu, Y. and Kong, X., Effects of three different nanomaterials on the properties and microstructure of sludge based geopolymers, Constr. Build. Mater., 414, 134965 (2024).
https://doi.org/10.1016/j.conbuildmat.2024.134965
Singh, R. and Budarayavalasa, S., Solidification and stabilization of hazardous wastes using geopolymers as sustainable binders, J. Mater. Cycles Waste Manage., 23(5), 1699-1725 (2021).
https://doi.org/10.1007/s10163-021-01245-0
Thomas, J., Thomas, P. S. and Stephen, R., Improved mechanical, thermal, and barrier properties of halloysite nanotubes and nanocellulose incorporated PVA-PEO films: For food packaging applications, Food Packag. Shelf Life, 46, 101373 (2024).
https://doi.org/10.1016/j.fpsl.2024.101373
Vignesh, J., Sivakumar, V. L., Kandasamy, A. and Al Khazaleh, M., Green engineering of surfactant-assisted nano silica dispersion in alkaline cementitious systems using chitosan, J. Environ. Nanotechnol., 14(3), 750-765 (2025a).
https://doi.org/10.13074/jent.2025.09.2531777
Vignesh, J., Sivakumar, V. L., Kandasamy, A. and Al Khazaleh, M., Bio-derived kraft lignin as a green stabilizer for surfactant-assisted nano silica dispersion in cementitious systems, J. Environ. Nanotechnol., 14(3), 766-780 (2025b).
https://doi.org/10.13074/jent.2025.09.2531781
Vilasini, P. P. and Thangasamy, L., Comparative long-term stabilization of pond ash using lime and cement: FTIR characterization, strength optimization and sustainable utilization, Next Mater., 8, 100908 (2025).
https://doi.org/10.1016/j.nxmate.2025.100908
Vilasini, P. P., Integrated mechanical, durability and environmental assessment of stabilized pond ash, Next Mater., 13, 102769 (2026).
https://doi.org/10.1016/j.nxmate.2026.102769
Walbrück, K., Maeting, F., Witzleben, S. and Stephan, D., Natural fiber-stabilized geopolymer foams—A review, Mater., 13(14), 3198 (2020).
https://doi.org/10.3390/ma13143198
Wang, P., Shi, M., Shu, Y., Niu, Q. and Zhang, P., Porous CaCO₃ fabricated by Ca-containing solid wastes for effective CO₂ adsorption, J. Environ. Chem. Eng., 13(2), 115815 (2025).
https://doi.org/10.1016/j.jece.2025.115815
Wang, Y., Liu, L., Ren, C., Ma, J., Shen, B., Zhao, P. and Zhang, Z., A novel amine functionalized porous geopolymer spheres from municipal solid waste incineration fly ash for CO₂ capture, J. Environ. Manage., 349, 119540 (2024).
https://doi.org/10.1016/j.jenvman.2023.119540
Xu, J., Kang, A., Wu, Z., Gong, Y. and Xiao, P., The effect of mechanical-thermal synergistic activation on the mechanical properties and microstructure of recycled powder geopolymer, J. Cleaner Prod., 327, 129477 (2021).
https://doi.org/10.1016/j.jclepro.2021.129477
Zhao, H., Hu, J., Wang, J., Zhou, L. and Liu, H., CO₂ capture by the amine-modified mesoporous materials, Acta Phys.-Chim. Sin., 23(6), 801-806 (2007).
