Apinya Kaoloun 1, Malinee Sriariyanun 1,2, Atthasit Tawai 1,2*, Saranya Sedtananun 3

1 Department of Chemical Engineering and Management, The Sirindhorn International Thai-German Graduate School of Engineering, King Mongkut’s University of Technology North Bangkok, Bangkok, Thailand

2 Biorefinery and Process Automation Engineering Center (BPAEC), King Mongkut’s University of Technology North Bangkok, Bangkok, Thailand

3 Department of Biotechnology, Faculty of Applied Science, King Mongkut’s University of Technology North Bangkok, Bangkok, Thailand

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ABSTRACT


Saponins exhibit significant potential in animal feed applications due to their roles in enhancing nutrient absorption and providing antimicrobial properties. However, conventional extraction methods using organic solvents pose potential health risks. This study proposes a sustainable extraction approach using deep eutectic solvents (DESs), a green solvent, to recover saponins from Camellia oleifera leaf waste, a food industry byproduct. Choline chloride (ChCl) and lactic acid (Lac) are selected as DES components, with response surface methodology (RSM) and genetic algorithm (GA) employed for process optimization. RSM achieves a saponin yield of 249.87 mg/g (raw material) at a ChCl-Lac ratio of 1:4, solid content of 17.5%, and pretreatment temperature of 57°C, while GA yields 232.17 mg/g at a ChCl-Lac ratio of 1:1, solid content of 21.5%, and pretreatment temperature of 54°C. Both DES extraction outperforms ethanol-based extraction (157.76 mg/g). Fermentation of hydrolysates produces ethanol concentrations of 6.14 mg/mL (RSM) and 7.07 mg/mL (GA), with yields of 42.35% and 41.58%, respectively, based on initial reducing sugar content. Minimal inhibition from residual saponins confirms the compatibility of DES-based pretreatment with fermentation. These findings establish DES-based extraction as a sustainable and efficient method for saponin recovery, with strong potential for integration into biorefinery applications, including bioethanol production.


Keywords: Bioethanol, Biorefinery, Deep eutectic solvents, Genetic algorithm, Response surface methodology, Saponin extraction.


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REFERENCES


  1. Bermúdez-Oria, A., Fernández-Prior, A., Castejón, M.L., Rodríguez-Gutiérrez, G., Fernández-Bolaños, J. 2023. Extraction of polyphenols associated with pectin from olive waste (alperujo) with choline chloride. Food Chemistry, 419, 136073.

  2. Chen, S., Kang, J., Zhu, H., Han, Z., Wang, L., Wang, K., Liu, J., Wu, Y., He, P., Tu, Y, Li, B. 2024. Tea seed saponins ameliorate cyclophosphamide-induced intestinal injury, immune disorder and gut microbial dysbiosis in mice. Food Bioscience, 57, 103504.

  3. Chuetor S., Panakkal E.J., Ruensodsai T., Cheenkachorn K., Kirdponpattara S., Cheng Y.S., Sriariyanun M. 2022. Improvement of enzymatic saccharification and ethanol production from rice straw using recycled ionic liquid: The effect of anti-solvent mixture, Bioengineering, 9, 115.

  4. Deng, Y., Wang, X., Zhang, C., Xie, P., Huang, L. 2024. Enhanced and green extraction of saponins from Gleditsia sinensis Lam. Pods by ultrasound-assisted deep eutectic solvents: optimization and comprehensive characterization. Food and Bioprocess Technology, 1–20.

  5. Duan, L., Dou, L.L., Guo, L., Li, P., Liu, E.H. 2016. Comprehensive evaluation of deep eutectic solvents in extraction of bioactive natural products. ACS Sustainable Chemistry Engineering, 4, 2405–2411.

  6. Guo, J., Zhao, N., Zhao, Y., Jin, H., Sun, G., Yu, J., Zhang, H., Shao, J., Yu, M., Yang, D., Liang, Z. 2024. The extraction using deep eutectic solvents and evaluation of tea saponin. Biology, 13, 438.

  7. Guo, N., Tong, T., Ren, N., Tu, Y., Li, B. 2018. Saponins from seeds of Genus Camellia: Phytochemistry and bioactivity. Phytochemistry, 149, 42–55.

  8. Hatzis C., Riley C., Philippidis G. 1996. Detailed material balance and ethanol yield calculations for the biomass-to-ethanol conversion process. Applied Biochemistry and Biotechnology, 57, 443–459.

  9. Hou, Y.J., Wang, P.W., Zhang, H., Fan, Y.Y., Cao, X., Luo, Y. Q., Li, Q., Njolibimi, M., Li, W., Hong, B, Zhao, C.J. 2024. A high-permeability method for extracting purple yam saponins based on ultrasonic-assisted natural deep eutectic solvent. Food Chemistry, 457, 140046.

  10. Im, K.H., Nguyen, T.K., Choi, J., Lee, T.S. 2016. Ethanol production from various sugars and cellulosic biomass by white rot fungus Lenzites betulinus. Mycobiology, 44, 48–53.

  11. Jose, D., Tawai, A., Divakaran, D., Bhattacharyya, D., Venkatachalam, P., Tantayotai, P., Sriariyanun, M. 2023. Integration of deep eutectic solvent in biorefining process of lignocellulosic biomass valorization. Bioresource Technology Reports, 21, 101365.

  12. Lei, J., Wang, Y., Li, W., Fu, S., Zhou, J., Lu, D., Wang, C., Sheng, X., Zhang, M., Xiao, S., Sun, C., Wang, G. 2022. Natural green deep eutectic solvents based eco-friendly and efficient extraction of flavonoids from Selaginella moellendorffii: Process optimization, composition identification and biological activity. Separation and Purification Technology, 283, 120203.

  13. Li, T., Zhang, H., Wu, C. E. 2014. Screening of antioxidant and antitumor activities of major ingredients from defatted Camellia oleifera seeds. Food science and biotechnology, 23, 873–880.

  14. Liu, X., Wu, Y., Gao, Y., Jiang, Z., Zhao, Z., Zeng, W., Mingyu, X., Liu, S., Liu, R., Chao, Y., Nie, S., Zhang, A., Li, C., Xiao, Z. 2024. Valorization of Camellia oleifera oil processing byproducts to value-added chemicals and biobased materials: A critical review. Green Energy and Environment, 9, 28–53.

  15. Ma, X., Gao, M., Yin, Z., Zhu, W., Liu, S., Wang, Q. 2020. Lactic acid and animal feeds production from Sophora flavescens residues by Rhizopus oryzae fermentation. Process biochemistry, 92, 401–408.

  16. Mavai, S., Bains, A., Sridhar, K., Chawla, P., Sharma, M. 2024. Emerging deep eutectic solvents for food waste valorization to achieve sustainable development goals: Bioactive extractions and food applications. Food Chemistry, 141000.

  17. Mujtaba M., Fraceto L.F., Fazeli M., Mukherjee S., Savassa S.M., Medeiros G.A., Pereira A.E.S., Mancini S.D., Lipponen J., Vilaplana F. 2023. Lignocellulosic biomass from agricultural waste to the circular economy: A review with focus on biofuels, biocomposites and bioplastics, Journal of Cleaner Production, 402, 136815.

  18. Sriariyanun M., Mutrakulcharoen P., Tepaamorndech S., Cheenkachorn K., Rattanaporn K. 2019. A rapid spectrophotometric method for quantitative determination of ethanol in fermentation products. Oriental Journal of Chemistry, 35, 744–750.

  19. Tang, Y., He, X., Sun, J., Liu, G., Li, C., Li, L., Sheng, J., Zhou, Z., Xin, M., Ling, D., Yi, P., Zheng, F., Li, J., Li, Z., Yang, Y., Tang, J., Chen, X. 2021. Comprehensive evaluation on tailor-made deep eutectic solvents (DESs) in extracting tea saponins from seed pomace of Camellia oleifera Abel. Food Chemistry, 342, 128243.

  20. Tsegaye, K.N., Alemnew, M., Berhane, N. 2024. Saccharomyces cerevisiae for lignocellulosic ethanol production: a look at key attributes and genome shuffling. Frontiers in Bioengineering and Biotechnology, 12, 1466644.

  21. Wei, Z., Zhang, W., Du, M., Zhong, H., Fang, X. 2024. Widely targeted metabolomic and KEGG analyses of natural deep eutectic solvent-based saponins extraction from Camellia oleifera Abel.: Effects on composition. Food Chemistry, 450, 139333.

  22. Wu, L., Chen, Z., Li, S., Wang, L., Zhang, J. 2021. Eco-friendly and high-efficient extraction of natural antioxidants from Polygonum aviculare leaves using tailor-made deep eutectic solvents as extractants. Separation and Purification Technology, 262, 118339.

  23. Wu R., Li Y., Wang X., Fu Y., Qin M., Zhang Y. 2023. In-situ lignin sulfonation for enhancing enzymatic hydrolysis of poplar using mild organic solvent pretreatment. Bioresource Technology, 369, 128410.

  24. Yu, X., Zhao, Z., Yan, X., Xie, J., Yu, Q., Chen, Y. 2023. Extraction optimization of tea saponins from Camellia oleifera seed meal with deep eutectic solvents: Composition identification and properties evaluation. Food Chemistry, 427, 136681.

  25. Yu, X.L., He, Y. 2018a. Development of a rapid and simple method for preparing tea-leaf saponins and investigation on their surface tension differences compared with tea-seed saponins. Molecules, 23, 1796.

  26. Yu, X.L., He, Y. 2018b. Optimization of tea‐leaf saponins water extraction and relationships between their contents and tea (Camellia sinensis) tree varieties. Food Science and Nutrition, 6, 1734–1740.

  27. Zhang, H., Li, X., Kang, M., Li, Z., Wang, X., Jing, X., Han, J. 2023. Sustainable ultrasound-assisted extraction of Polygonatum sibiricum saponins using ionic strength-responsive natural deep eutectic solvents. Ultrasonics Sonochemistry, 100, 106640.

  28. Zhang, P., Xiong, Y., Bi, L., Zhong, H., Ren, J., Zhou, B. 2024. Non-antibiotic feed additives production by Acremonium terricola solid-fermented Camellia oleifera meal. Bioresources and Bioprocessing, 11, 90.

  29. Zhao, Y., Su, R., Zhang, W., Yao, G. L., Chen, J. 2020. Antibacterial activity of tea saponin from Camellia oleifera shell by novel extraction method. Industrial crops and products, 153, 112604.


ARTICLE INFORMATION


Received: 2025-02-21
Revised: 2025-04-17
Accepted: 2025-04-29
Available Online: 2025-05-23


Cite this article:

Kaoloun A., Sriariyanun M., Tawai A., Sedtananun S. 2025. Simultaneous green extraction of tea saponins
from Camellia oleifera leaf waste using deep eutectic solvents for potential animal feed and bioethanol applications. International Journal of Applied Science and Engineering, 22, 2025056.  https://doi.org/10.6703/IJASE.202506_22(2).002

  Copyright The Author(s). This is an open access article distributed under the terms of the Creative Commons Attribution License (CC BY 4.0), which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are cited.