Abstract
Sugarcane bagasse, a major by-product from cane sugar industry contains mainly cellulose, lignin and hemicellulose which can be fractionated and used for further products. In this study, an organosolv fractionation based on formic acid was used to pretreat the sugarcane bagasse, separate, and recover cellulose. A central-composite matrix with three independent variables (formic acid concentration, temperature, and fractionation time) was designed to study their simultaneous effects on the delignification, purity of recovered cellulose. Temperature was found to be the main factor affecting the fractionation process, following the formic acid concentration and fractionation time. The fractionation process removed not only lignin and hemicellulose from sugarcane bagasse but also altered the crystallinity of cellulose to facilitate the glucan hydrolysis. The fractionation temperature and delignification were inversely proportional to the crystallinity of the recovered cellulose (R2 = 0.99 and 0.83, respectively), regardless the formic acid concentration used. There was a strong linear correlation between delignification and hydrolysis ability of the fractionated glucan. The formic acid-based fractionation removed 90.6% lignin, resulted in recovered relatively pure cellulose with 92.3% glucan which enzymatic saccharification ability was achieved 91.4% to produce fermentable sugars.
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
Data Availability
The authors declare that all data supporting the findings of this study is available in this manuscript.
References
Ahmad, N. and M.R. Zakaria. 2019. Chapter 8 - Oligosaccharide From Hemicellulose In Lignocellulose for Future Bioeconomy, ed. Ariffin, H., Sapuan, S. M., Hassan, M. A., pp. 135–52: Elsevier.
Chandel, A.K., S.S. da Silva, W. Carvalho, and O.V. Singh. 2012. Sugarcane bagasse and leaves: Foreseeable biomass of biofuel and bio-products. Journal of Chemical Technology and Biotechnology 87: 11–20. https://doi.org/10.1002/jctb.2742.
Chotirotsukon, C., M. Raita, M. Yamada, H. Nishimura, T. Watanabe, N. Laosiripojana, and V. Champreda. 2021. Sequential fractionation of sugarcane bagasse using liquid hot water and formic acid-catalyzed glycerol-based organosolv with solvent recycling. BioEnergy Research 14: 135–152. https://doi.org/10.1007/s12155-020-10181-0.
Dapía, S., V. Santos, and J.C. Parajó. 2002. Study of formic acid as an agent for biomass fractionation. Biomass and Bioenergy 22: 213–21. https://doi.org/10.1016/S0961-9534(01)00073-3.
Erfani Jazi, M., G. Narayanan, F. Aghabozorgi, B. Farajidizaji, A. Aghaei, M.A. Kamyabi, C.M. Navarathna, and T.E. Mlsna. 2019. Structure, chemistry and physicochemistry of lignin for material functionalization. SN Applied Sciences 1: 1094. https://doi.org/10.1007/s42452-019-1126-8.
Huang, R.L., W. Qi, R.X. Su, and Z.M. He. 2010. The optimization of fractionating lignocellulose by formic acid using response surface methodology. Energy Sources, Part A: Recovery, Utilization, and Environmental Effects 32: 1282–1292. https://doi.org/10.1080/15567030903076669.
Imman, S., P. Khongchamnan, W. Wanmolee, N. Laosiripojana, T. Kreetachat, C. Sakulthaew, C. Chokejaroenrat, and N. Suriyachai. 2021. Fractionation and characterization of lignin from sugarcane bagasse using a sulfuric acid catalyzed solvothermal process. RSC Advances 11: 26773–26784. https://doi.org/10.1039/D1RA03237B.
Khaleghipour, L., J.A. Linares-Pastén, H. Rashedi, S.O. Ranaei Siadat, A. Jasilionis, S. Al-Hamimi, R.R.R. Sardari, and E.N. Karlsson. 2021. Extraction of sugarcane bagasse arabinoxylan, integrated with enzymatic production of xylo-oligosaccharides and separation of cellulose. Biotechnology for Biofuels 14: 153. https://doi.org/10.1186/s13068-021-01993-z.
Kupiainen, L., J. Ahola, and J. Tanskanen. 2012. Hydrolysis of organosolv wheat pulp in formic acid at high temperature for glucose production. Bioresource Technology 116: 29–35. https://doi.org/10.1016/j.biortech.2012.04.012.
Lee, S.H., T.V. Doherty, R.J. Linhardt, and J.S. Dordick. 2009. Ionic liquid-mediated selective extraction of lignin from wood leading to enhanced enzymatic cellulose hydrolysis. Biotechnology and Bioengineering 102: 1368–1376. https://doi.org/10.1002/bit.22179.
Leite, R., Y.M.B.D. Almeida, S.M. Sarmento, K.G.B. Alves, E.F.D. Melo, and R.M. Souto-Maior. 2016. Solvent-fractionated sugar cane bagasse lignin: structural characteristics and electro-spinnability. e-Polymers 16: 137–44. https://doi.org/10.1515/epoly-2015-0229.
Masarin, F., D. Gurpilhares, D. Baffa, M. Barbosa, W. Carvalho, A. Ferraz, and A. Milagres. 2011. Chemical composition and enzymatic digestibility of sugarcane clones selected for varied lignin content. Biotechnology for Biofuels 4: 55.
Mesa, L., E. González, C. Cara, M. González, E. Castro, and S.I. Mussatto. 2011. The effect of organosolv pretreatment variables on enzymatic hydrolysis of sugarcane bagasse. Chemical Engineering Journal 168: 1157–1162. https://doi.org/10.1016/j.cej.2011.02.003.
Neubert, L., J. Sunthornvarabhas, M. Sakulsombat, and K. Sriroth. 2020. Delignification and fractionation of sugarcane bagasse with ionic liquids. Cellulose Chemistry and Technology 54: 301–18. https://doi.org/10.35812/CelluloseChemTechnol.2020.54.32.
Ngo, D.S., K.A. To, and T.A. Pham. 2016. Comparision of ethanol yield between separate and simultaneous hydrolysis and ethanol fermentation of formic-fractionated sugar cane bagasse. Vietnam Journal of Science and Technology 54: 222. https://doi.org/10.15625/2525-2518/54/2A/11934.
Peng, F., J.-L. Ren, F. Xu, J. Bian, P. Peng, and R.-C. Sun. 2009. Comparative study of hemicelluloses obtained by graded ethanol precipitation from sugarcane bagasse. Journal of Agricultural and Food Chemistry 57: 6305–6317. https://doi.org/10.1021/jf900986b.
Rahikainen, J.L., R. Martin-Samedro, H. Heikkinen, S. Rovio, K. Marjamaa, T. Tamminen, O.J. Rojas, and K. Kruus. 2013. Inhibitory effect of lignin during cellulose bioconversion: The effect of lignin chemistry on non-productive enzyme adsorption. Bioresource Technology 133: 270–278.
Segal, L., J.J. Creely, T. Martin, and C.M. Conrad. 1959. An empirical method for estimationg the degree of crystallinity of native cellulose using the X-ray diffractometer. Textile Research Journal 29: 786–794. https://doi.org/10.1177/004051755902901003.
Selig, M., N. Weiss and Y. Ji. 2008. Enzymatic saccharification of lignocellulosic biomass. Technical report NREL/TP-510-42629. National Renewable Energy Laboratory.
Sindhu, R., P. Binod, K. Satyanagalakshmi, K.U. Janu, K.V. Sajna, N. Kurien, R.K. Sukumaran, and A. Pandey. 2010. Formic acid as a potential pretreatment agent for the conversion of sugarcane bagasse to bioethanol. Applied Biochemistry and Biotechnology 162: 2313–2323. https://doi.org/10.1007/s12010-010-9004-2.
Siqueira, G., A. Várnai, A. Ferraz, and A.M.F. Milagres. 2013. Enhancement of cellulose hydrolysis in sugarcane bagasse by the selective removal of lignin with sodium chlorite. Applied Energy 102: 399–402. https://doi.org/10.1016/j.apenergy.2012.07.029.
Sluiter, A., B. Hames, R. Ruiz, C. Scarlata, J. Sluiter, D. Templeton and D. Crocker. 2011. Determination os structural carbohydrates and lignin in biomass. Technical Report NREL/TP-510–42618. National Renewable Energy Laboratory.
Snelders, J., E. Dornez, B. Benjelloun-Mlayah, W.J.J. Huijgen, P.J. de Wild, R.J.A. Gosselink, J. Gerritsma, and C.M. Courtin. 2014. Biorefining of wheat straw using an acetic and formic acid based organosolv fractionation process. Bioresource Technology 156: 275–282. https://doi.org/10.1016/j.biortech.2014.01.069.
Suriyachai, N., V. Champreda, N. Kraikul, W. Techanan, and N. Laosiripojana. 2018. Fractionation of lignocellulosic biopolymers from sugarcane bagasse using formic acid-catalyzed organosolv process. Biotech 8: 221. https://doi.org/10.1007/s13205-018-1244-9.
Tan, Y.T., A.S.M. Chua, and G.C. Ngoh. 2020. Deep eutectic solvent for lignocellulosic biomass fractionation and the subsequent conversion to bio-based products—A review. Bioresource Technology 297: 122522. https://doi.org/10.1016/j.biortech.2019.122522.
Tu, Q., S. Fu, H. Zhan, X. Chai, and L.A. Lucia. 2008. Kinetic modeling of formic acid pulping of bagasse. Journal of Agricultural and Food Chemistry 56: 3097–3101. https://doi.org/10.1021/jf0729659.
Wildschut, J., A.T. Smit, J.H. Reith, and W.J. Huijgen. 2013. Ethanol-based organosolv fractionation of wheat straw for the production of lignin and enzymatically digestible cellulose. Bioresource Technology 135: 58–66. https://doi.org/10.1016/j.biortech.2012.10.050.
Xu, J., C. Li, L. Dai, C. Xu, Y. Zhong, F. Yu, and C. Si. 2020. Biomass fractionation and lignin fractionation towards lignin valorization. Chemsuschem 13: 4284–4295. https://doi.org/10.1002/cssc.202001491.
Yang, B., Z. Dai, S.-D. Ding, and C. Wyman. 2011. Enzymatic Hydrolysis of Cellulosic Biomass. Biofules 2: 421–450.
Zeng, J., D. Singh, D. Gao, and S. Chen. 2014. Effects of lignin modification on wheat straw cell wall deconstruction by Phanerochaete chrysosporium. Biotechnology for Biofuels 7: 161. https://doi.org/10.1186/s13068-014-0161-3.
Zhang, M., W. Qi, R. Liu, R. Su, S. Wu, and Z. He. 2010. Fractionating lignocellulose by formic acid: Characterization of major components. Biomass and Bioenergy 34: 525–532. https://doi.org/10.1016/j.biombioe.2009.12.018.
Zhao, X., and D. Liu. 2012. Fractionating pretreatment of sugarcane bagasse by aqueous formic acid with direct recycle of spent liquor to increase cellulose digestibility-the Formiline process. Bioresource Technology 117: 25–32. https://doi.org/10.1016/j.biortech.2012.04.062.
Zhao, X., K. Cheng, and D. Liu. 2009. Organosolv pretreatment of lignocellulosic biomass for enzymatic hydrolysis. Applied Microbiology and Biotechnology 82: 815–827. https://doi.org/10.1007/s00253-009-1883-1.
Acknowledgements
This research was support in part by the Grant DT.05.13/NLSH. The authors are graceful of Ministry of Industry and Trade (MOIT), Bio-energy program for financial support.
Author information
Authors and Affiliations
Contributions
Duy Sa Ngo: experimental procedures. Kim Anh To: experimental procedures, reviewing the manuscript. Tuan Anh Pham: data preparation and interpretation, writing the manuscript, funding acquisition. All authors read and approved the final manuscript.
Corresponding author
Ethics declarations
Conflict of interest
The authors have no conflict of interst to declare.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
About this article
Cite this article
Pham, T.A., Ngo, D.S. & To, K.A. Formic Acid-Based Organosolv Delignification of Sugarcane Bagasse for Efficient Enzymatic Saccharification. Sugar Tech 24, 779–787 (2022). https://doi.org/10.1007/s12355-022-01114-6
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s12355-022-01114-6