Adsorption Kinetics and Process Parameter Effects on Oil Uptake by Tamarind Fruit-Shell Activated Carbon

Lusi Ernawati; Eka Masrifatus Anifah; Musyarofah Musyarofah; Mutia Reza; Joko Waluyo; Norzahir Sapawe

doi:10.33795/jtkl.v9i2.7596

Authors

Lusi Ernawati Department of Chemical Engineering, Institut Teknologi Kalimantan, Jl. Soekarno Hatta KM 15, Balikpapan, Kalimantan Timur, 76127, Indonesia
Eka Masrifatus Anifah Department of Environmental Engineering, Institut Teknologi Kalimantan, Jl. Soekarno Hatta KM 15, Balikpapan, Kalimantan Timur, 76127, Indonesia
Musyarofah Musyarofah Department of Physics, Institut Teknologi Kalimantan, Jl. Soekarno Hatta KM 15, Balikpapan, Kalimantan Timur, 76127, Indonesia
Mutia Reza Department of Chemical Engineering, Institut Teknologi Kalimantan, Jl. Soekarno Hatta KM 15, Balikpapan, Kalimantan Timur, 76127, Indonesia
Joko Waluyo Department of Chemical Engineering, Faculty of Engineering, Universitas Sebelas Maret, Jl. Ir. Sutami No. 36A, Kentingan, Surakarta, 57126, Indonesia
Norzahir Sapawe Universiti Kuala Lumpur Branch Campus Malaysian Institute of Chemical and Bioengineering Technology (UniKL MICET), Lot 1988 Vendor City, Taboh Naning, 78000 Alor Gajah, Melaka, Malaysia

DOI:

https://doi.org/10.33795/jtkl.v9i2.7596

Keywords:

activated-carbon, adsorption, chemical activation, isotherm, lubricant oil, tamarind shell

Abstract

Oil contamination presents a major challenge to wastewater treatment systems due to its detrimental effects. This research explores the effectiveness of activated carbon derived from tamarind fruit shells as an adsorbent for removing oil from wastewater. The activated carbon was prepared using three different chemical agents: phosphoric acid, zinc chloride, and sodium hydroxide. Characterization of the resulting carbon materials was performed using XRD, FTIR, SEM, and BET analysis. Batch adsorption experiments were conducted to evaluate the influence of initial oil concentration, adsorbent dosage, contact time, temperature, and pH. The BET specific surface area, pore size and total pore volume for the optimum adsorption capacity of activated carbon using H₃PO₄ are obtained at 617.59 m².g^-1, 37.14 cm³.g^-1 and 0.812 g.g^-1, respectively. Optimal adsorption occurred at an oil concentration of 5000 mg.L^-1, a dosage of 1 g.L^-1, a contact time of 60 minutes, a temperature of 60°C, and neutral pH (7). Across all activating agents, the Langmuir isotherm best described the adsorption equilibrium, while adsorption kinetics followed the pseudo-second-order model. Among the samples, activated carbon treated with H₃PO₄ demonstrated the highest adsorption capacity (1070 mg.g^-1), followed by ZnCl₂ (879 mg.g^-1), and NaOH (643 mg.g^-1). These results indicate that tamarind shell-derived activated carbon is a cost-effective and efficient solution for oil removal in wastewater treatment applications.

References

M. L. Chan, Frost & Sullivan’s 2024 ASEAN Automotive Growth Outlook, https://store.frost.com/frost-sullivan-s-2024-asean-automotive-growth-outlook.html.

ASEAN Automotive Federation (AAF), Asean Automotive Federation 2023 Statistics, https://www.asean-autofed.com/.

D. Susilo, Macro Environment Analysis of Automotive Industry in Indonesia, BISE: Jurnal Pendidikan Bisnis dan Ekonomi, vol. 4, no. 2, pp. 150–158, 2018.

J. Guo, C. Wang, Analysis of Contaminants in Vehicle Maintenance and Repair Enterprise, Advances in Engineering Research, vol. 159, pp. 228–232, 2018.

P. Singh, V. Kadam, Y. Patil, Isolation and development of a microbial consortium for the treatment of automobile service station wastewater, J. Appl. Microbiol, vol. 132, no. 2, pp. 1048–1061, 2022.

M. Bujang, N. A. Ibrahim, A. Eh Rak, Physicochemical quality of oily wastewater from automotive workshop in Kota Bharu, Kelantan Malaysia, Aust. J. Basic Appl. Sci., vol. 6, no. 9, pp. 748–752, 2012.

H. S. Abd El-Gawad, Oil and Grease Removal from Industrial Wastewater Using New Utility Approach, Advances in Environmental Chemistry, vol. 2014, p. 16878, 2014.

S. Putatunda, S. Bhattacharya, D. Sen, C. Bhattacharjee, A review on the application of different treatment processes for emulsified oily wastewater, Int. J. Environ. Sci. Technol., vol. 16, pp. 2525–2536, 2019.

A. Bhattacharyya, L. Liu, K. Lee, J. Miao, Review of Biological Processes in a Membrane Bioreactor (MBR): Effects of Wastewater Characteristics and Operational Parameters on Biodegradation Efficiency When Treating Industrial Oily Wastewater, J. Mar. Sci. Eng., vol. 10, no. 9, p. 1229, 2022.

H. J. Tanudjaja, C. A. Hejase, V. V. Tarabara, A. G. Fane, J. W. Chew, Membrane-based separation for oily wastewater: A practical perspective, Water Research, vol. 156, pp. 347–365, 2019.

Y. Sun, H. Li, G. Li, B. Gao, Q. Yue, X. Li, Characterization and coagulation behavior of polymeric aluminum ferric silicate for high-concentration oily wastewater treatment, Chem. Eng. Res. Des., vol. 119, pp. 23–32, 2017.

M. A. H. Aswadi, M. A. Shukor, M. A. Ishak, Kinetics and Effects of Process Parameters on Oil Adsorption using Activated Carbon from Rubber Seed Kernels (Hevea brasiliensis), Chem. Eng. Trans., vol. 106, pp. 991–996, 2023.

H. J. Al-Jaaf, N. S. Ali, S. M. Alardhi, T. M. Albayati, Implementing eggplant peels as an efficient bio-adsorbent for treatment of oily domestic wastewater, Desalination Water Treat, vol. 245, pp. 91–100, 2022.

S. Martini, S. Afroze, K. A. Roni, Modified eucalyptus bark as a sorbent for simultaneous removal of COD, oil, and Cr(III) from industrial wastewater, Alexandria Engineering Journal, vol. 59, no. 3, pp. 1857–1867, 2020.

N. S. M. Thani, R. M. Ghazi, N. Ismail, Response Surface Methodology Optimization of Oil Removal Using Banana Peel as Bisorbent, Malaysian Journal of Analytical Science, vol. 21, no. 5, pp. 1125–1134, 2017. doi: 10.17576/mjas-2017-2105-12.

D. Peng, S. Cheng, H. Li, X. Guo, Effective multi-functional biosorbent derived from corn stalk pith for dyes and oils removal, Chemosphere, vol. 272, p. 129963, 2021.

J. S. Vaza, S. A. Bhalerao, Biosorption of Zinc (II) from Aqueous Solution using Tartaric Acid Modified Tamarind (Tamarindus indica L.) Pod Shell Powder, Int. J. Res. Appl. Sci. Eng. Technol., vol. 7, no. 1, pp. 500–514, 2019.

S. L. Pandharipande, R. P. Kalnake, Tamarind Fruit Shell Adsorbent Synthesis, Characterization and Adsorption Studies for Removal of Cr(VI) & Ni(II) Ions from Aqueous Solution, Int. J. Eng. Sci. Emerg. Technol., vol. 4, no. 2, pp: 83–89, 2013.

P. G. Radhakrishnan, S. P. Varghese, B. C Das, Application of ethylenediamine hydroxypropyl tamarind fruit shell as adsorbent to remove Eriochrome black T from aqueous solutions – Kinetic and equilibrium studies, Separation Science and Technology (Philadelphia), vol. 53, no. 3, pp. 417–438, 2018.

V. Sivasankar, S. Rajkumar, S. Murugesh, A. Darchen, Tamarind (Tamarindus indica) fruit shell carbon: A calcium-rich promising adsorbent for fluoride removal from groundwater, J. Hazard. Mater., vol. 225–226, pp. 164–172, 2012.

Y. Sun, H. Li, G. Li, B. Gao, Q. Yue, X. Li, Characterization and ciprofloxacin adsorption properties of activated carbons prepared from biomass wastes by H3PO4 activation, Bioresour. Technol., vol. 217, pp. 239–244, 2016.

A. Toprak, T. Kopac, Carbon Dioxide Adsorption Using High Surface Area Activated Carbons from Local Coals Modified by KOH, NaOH and ZnCl2 Agents, Int. J. Chem. React. Eng., vol. 15, no. 3, p. 20160042, 2017.

J. Bayuo, K. B. Pelig-ba, M. A. Abukari, Isotherm Modeling of Lead (II) Adsorption from Aqueous Solution Using Groundnut Shell as a Low-Cost Adsorbent, IOSR Journal of Applied Chemistry, vol. 11, no. 11, pp. 18–23, 2018.

J. O. Nwadiogbu, V. I. E. Ajiwe, P. A. C. Okoye, Removal of crude oil from aqueous medium by sorption on hydrophobic corncobs: Equilibrium and kinetic studies, Journal of Taibah University for Science, vol. 10, no. 1, pp. 56–63, 2016.

E. Piperopoulos, L. Calabrese, E. Mastronardo, S. H. A. Rahim, E. Proverbio, C. Milone, Assessment of sorption kinetics of carbon nanotube-based composite foams for oil recovery application, J. Appl. Polym. Sci., vol. 136, no. 14, p. 47374, 2019.

L. Ernawati, M. Reza, A. C. Synthia, D. A. Kartikasari, I. K. Maharsih, A. Halim, Role of Chemical Activating Agent on the Characteristics of Activated Carbon Derived from Fruit-Peel Waste for Aqueous Dye Removal, Key Engineering Materials, vol. 937, pp. 165–180, 2022.

A. Halim, L. Ernawati, M. Ismayati, F. Martak, T. Enomae, Bioinspired cellulose-based membranes in oily wastewater treatment, Front. Environ. Sci. Eng., vol. 16, no. 7, p. 94, 2022.

O. Oginni, K. Singh, G. Oporto, B. Dawson-Andoh, L. McDonald, E. Sabolsky, Effect of one-step and two-step H3PO4 activation on activated carbon characteristics, Bioresour. Technol. Rep., vol. 8, p. 100307, 2019.

S. M. Villota, H. Lei, E. Villota, M. Qian, J. Lavarias, V. Taylan, I. Agulto, W. Mateo, M. Valentin, M. Denson, Microwave-Assisted Activation of Waste Cocoa Pod Husk by H3PO4 and KOH–Comparative Insight into Textural Properties and Pore Development, ACS Omega, vol. 4, no. 4, pp. 7088–7095, 2019.

J. Xu, L. Chen, H. Qu, Y. Jiao, J. Xie, G. Xing, Preparation and characterization of activated carbon from reedy grass leaves by chemical activation with H3PO4, Appl. Surf. Sci., vol. 320, pp. 674–680, 2014.

B. Li, J. Hu, H. Xiong, Y. Xiao, Application and Properties of Microporous Carbons Activated by ZnCl2: Adsorption Behavior and Activation Mechanism, ACS Omega, vol. 5, no. 16, pp. 9388–9397, 2020.

J. Guo, A. C. Lua, Textural and chemical properties of adsorbent prepared from palm shell by phosphoric acid activation, Mater. Chem. Phys., vol. 80, no. 1, pp. 114–119, 2003.

I. A. W. Tan, A. L. Ahmad, B. H. Hameed, Preparation of activated carbon from coconut husk: Optimization study on removal of 2,4,6-trichlorophenol using response surface methodology, J. Hazard. Mater., vol. 153, no. 1–2, pp. 709–717, 2008.

A. Ahmadpour, D. D. Do, The preparation of activated carbon from macadamia nutshell by chemical activation, Carbon, vol. 35, no. 12, pp. 1723–1732, 1997.

P. González-García, Activated carbon from lignocellulosics precursors: A review of the synthesis methods, characterization techniques and applications, Renew. Sustain. Energy Rev., vol. 82, pp. 1393–1414, 2018.

K. Okiel, M. El-Sayed, M. Y. El-Kady, Treatment of oil–water emulsions by adsorption onto activated carbon, bentonite and deposited carbon, Egyptian Journal of Petroleum, vol. 20, no. 2, pp. 9–15, 2011.

R. Asadpour, N. B. Sapari, M. H. Isa, K. U. Orji, Enhancing the hydrophobicity of mangrove bark by esterification for oil adsorption, Water Science and Technology, vol. 70, no. 7, pp. 1220–1228, 2014.

M. Fathy, M. El-Sayed, M. Ramzi, O. H. Abdelraheem, Adsorption separation of condensate oil from produced water using ACTF prepared of oil palm leaves by batch and fixed bed techniques, Egyptian Journal of Petroleum, vol. 27, no. 3, pp. 319–326, 2018.

U. A. Abel, G. R. Habor, O. I. Oseribho, Adsorption Studies of Oil Spill Clean-up Using Coconut Coir Activated Carbon (CCAC), American Journal of Chemical Engineering, vol. 8, no. 2, pp. 36–47, 2020.

S. Saruchi, B. S. Kaith, R. Jindal, V. Kumar, The adsorption of crude oil from an aqueous solution using a Gum tragacanth polyacrylic acid based hydrogel, Pet. Sci. Technol., vol. 33, no. 3, pp. 278–286, 2015.

W. Pitakpoolsil, M. Hunsom, Treatment of biodiesel wastewater by adsorption with commercial chitosan flakes: Parameter optimization and process kinetics, J. Environ. Manage., vol. 133, pp. 284–292, 2014.

A. K. Fard, G. Mckay, Y. Manawi, Z. Malaibari, M. A. Hussien, Outstanding adsorption performance of high aspect ratio and super-hydrophobic carbon nanotubes for oil removal, Chemosphere, vol. 164, pp. 142–155, 2016.

S. S. Elanchezhiyan, S. M. Prabhu, S. Meenakshi, Effective adsorption of oil droplets from oil-in-water emulsion using metal ions encapsulated biopolymers: Role of metal ions and their mechanism in oil removal, Int. J. Biol. Macromol., vol. 112, pp. 294–305, 2018.

K. AlAmeri, A. Giwa, L. Yousef, A. Alraeesi, H. Taher, Sorption and removal of crude oil spills from seawater using peat-derived biochar: An optimization study, J. Environ. Manage., vol. 250, p. 109465, 2019.

O. Abdelwahab, Assessment of raw luffa as a natural hollow oleophilic fibrous sorbent for oil spill cleanup, Alexandria Engineering Journal, vol. 53, no. 1, pp. 213–218, 2014.

S. E. Agarry, K. M. Oghenejoboh, E. O. Oghenejoboh, C. N. Owabor, O. O. Ogunleye, Adsorptive remediation of crude oil contaminated marine water using chemically and thermally modified coconut (Cocos nucifera) husks, Journal of Environmental Treatment Techniques, vol. 8, no. 2, pp. 694–707, 2020.

A. Amari, H. S. K. Alawameleh, M. Isam, M. A. J. Maktoof, H. Osman, B. Panneerselvam, M. Thomas, Thermodynamic Investigation and Study of Kinetics and Mass Transfer Mechanisms of Oily Wastewater Adsorption on UIO-66–MnFe2O4 as a Metal–Organic Framework (MOF), Sustainability, vol. 15, no. 3, p. 2488, 2023.

R. Wahi, L. A. Chuah, T. S. Y. Choong, Z. Ngaini, M. M. Nourouzi, Oil removal from aqueous state by natural fibrous sorbent: An overview, Sep. Purif. Technol., vol. 113, pp. 51–63, 2013.

T. H. Nazifa, T. Hadibarata, A. Yuniarto, M. S. Elshikh, A. Syafiuddin, Equilibrium, kinetic and thermodynamic analysis petroleum oil adsorption from aqueous solution by magnetic activated carbon, IOP Conference Series: Materials Science and Engineering, vol. 495, p. 012060, 2019.

A. El Shahawy, G. Heikal, Organic pollutants removal from oily wastewater using clean technology economically, friendly biosorbent (Phragmites australis), Ecol. Eng., vol. 122, pp. 207–218, 2018.

Y. Li, M. Wang, D. Sun, Y. Li, T. Wu, Effective removal of emulsified oil from oily wastewater using surfactant-modified sepiolite, Appl. Clay Sci., vol. 157, pp. 227–236, 2018.

S. S. D. Elanchezhiyan, S. Meenakshi, Facile Fabrication of Metal Ions-Incorporated Chitosan/β-Cyclodextrin Composites for Effective Removal of Oil from Oily Wastewater, ChemistrySelect, vol. 2, no. 35, pp. 11393–11401, 2017.

H. J. Choi, Agricultural bio-waste for adsorptive removal of crude oil in aqueous solution, J. Mater. Cycles Waste Manag., vol. 21, pp. 356–364, 2019.

M. J. A. Alatabe, H. A. Faris, H. Husham, Natural Biosorbent for Oil Adsorption from Produced Water by Sedge Cane, J. Ecol. Eng., vol. 24, no. 10, pp. 67–76, 2023.

K. G. Akpomie, C. C. Ezeofor, J. U. Ani, S. I. Eze, C. C. Odo, E. A. Onoabedje, Equilibrium isotherms modeling of crude oil sorption from aqua mixture onto Codiaeum variegatum stem powder, Pet. Sci. Technol., vol. 37, no. 3, pp. 329–336, 2019.

S. Songsaeng, P. Thamyongkit, S. Poompradub, Natural rubber/reduced-graphene oxide composite materials: Morphological and oil adsorption properties for treatment of oil spills, J. Adv. Res., vol. 20, pp. 79–89, 2019.

K. G. Akpomie, J. Conradie, Treatment of motor oil-contaminated water via sorption onto natural organic lignocellulosic waste: thermodynamics, kinetics, isotherm, recycling, and reuse, Biomass Convers. Biorefin., vol. 13, pp. 10285–10297, 2023.

J.-Q. Hu, S.-Z. Yang, L. Guo, X. Xu, T. Yao, F. Xie, Microscopic investigation on the adsorption of lubrication oil on microplastics, J. Mol. Liq., vol. 227, pp. 351–355, 2017.

N. Lv, X. Wang, S. Peng, H. Zhang, L. Luo, Study of the kinetics and equilibrium of the adsorption of oils onto hydrophobic jute fiber modified via the sol-gel method, Int. J. Environ. Res. Public Health, vol. 15, no. 5, p. 969, 2018.

S. Saruchi, V. Kumar, Separation of crude oil from water using chitosan based hydrogel, Cellulose, vol. 26, pp. 6229–6239, 2019.