Abstract
The use of endoglucanase enzymes as pretreatment of high-yield pulps to produce lignocellulose nanofibrils (LCNFs) has garnered increasing interest at both industrial and scientific levels. However, the lignin present in the lignocellulosic fibers hinders the enzymatic treatment reducing the efficiency of the further fibrillation process. This work postulates that modifying the structure of the residual lignin in the pulp can help to improve LCNF production. Laccase-mediator system (LMS) was evaluated to promote lignin oxidation of pressurized groundwood pulp from Pinus radiata previous to a treatment with endoglucanases and mechanical refining to produce LCNFs. As a result, it was observed that the LMS treatment improved the accessibility of the endoglucanase enzyme in the fibers, increasing their efficiency. Furthermore, it was observed a reduction in residual lignin and an increment in acidic groups in the LMS treated pulps facilitated the mechanical fibrillation process, enabling the production of LCNFs with a high aspect ratio. It was also observed that the pulps treated with a laccase-endoglucanase combination allowed to production of LCNF suspensions with zeta potential values sufficient for the nanofibrils not to form aggregates and to be considered stable (< − 25 mV).
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References
Aguayo MG, Quintupill L, Castillo R et al (2010) Determination of differences in anatomical and chemical characteristics of tension and opposite wood of 8-year old Eucalyptus globulus. Maderas Ciencia y Tecnologia 12:241–251
Albornoz-Palma G, Betancourt F, Mendonça RT et al (2020a) Relationship between rheological and morphological characteristics of cellulose nanofibrils in dilute dispersions. Carbohydr Polym 230:115588. https://doi.org/10.1016/j.carbpol.2019.115588
Albornoz-Palma G, Ching D, Valerio O et al (2020b) Effect of lignin and hemicellulose on the properties of lignocellulose nanofibril suspensions. Cellulose 27:10631–10647. https://doi.org/10.1007/s10570-020-03304-5
Albornoz-Palma G, Ortega-Sanhueza I, Teruel-Juanes R et al (2023a) Understanding the effect of lignin on the production process and characteristics of lignocellulose nanofibrils from Eucalyptus nitens. Cellulose 30:6811–6831. https://doi.org/10.1007/s10570-023-05299-1
Albornoz-Palma G, Ortega-Sanhueza I, Teruel-Juanes R et al (2023b) Effect of lignin on the morphological, rheological, and dielectric characteristics of lignocellulose nanofibrils from Pinus radiata. Ind Crops Prod 204:117323. https://doi.org/10.1016/j.indcrop.2023.117323
Andrade A, Henríquez-Gallegos S, Albornoz-Palma G, Pereira M (2021) Effect of the chemical and structural characteristics of pulps of Eucalyptus and Pinus on the deconstruction of the cell wall during the production of cellulose nanofibrils. Cellulose 28:5387–5399. https://doi.org/10.1007/s10570-021-03848-0
Arantes V, Dias IKR, Berto GL et al (2020) The current status of the enzyme-mediated isolation and functionalization of nanocelluloses: production, properties, techno-economics, and opportunities. Cellulose 27:10571–10630. https://doi.org/10.1007/s10570-020-03332-1
Bian H, Gao Y, Luo J et al (2019) Lignocellulosic nanofibrils produced using wheat straw and their pulping solid residue: From agricultural waste to cellulose nanomaterials. Waste Manag 91:1–8. https://doi.org/10.1016/j.wasman.2019.04.052
Chen Q, Marshall MN, Geib SM et al (2012) Effects of laccase on lignin depolymerization and enzymatic hydrolysis of ensiled corn stover. Bioresour Technol 117:186–192. https://doi.org/10.1016/j.biortech.2012.04.085
Chio C, Sain M, Qin W (2019) Lignin utilization: a review of lignin depolymerization from various aspects. Renew Sustain Energy Rev 107:232–249. https://doi.org/10.1016/j.rser.2019.03.008
Christopher LP, Yao B, Ji Y (2014) Lignin biodegradation with Laccase–Mediator systems. Front Energy Res 2:234. https://doi.org/10.3389/fenrg.2014.00012
Delgado-Aguilar M (2015) Nanotecnología en el sector papelero: mejoras en calidad y permanencia de las fibras de alto rendimiento y secundarias en una economía circular mediante el uso de nanofibras y el refino enzimático. Universitat de Girona
Delgado-Aguilar M, González I, Tarrés Q et al (2016) The key role of lignin in the production of low-cost lignocellulosic nanofibres for papermaking applications. Ind Crops Prod 86:295–300. https://doi.org/10.1016/j.indcrop.2016.04.010
Dias MC, Belgacem MN, de Resende JV et al (2022) Eco-friendly laccase and cellulase enzymes pretreatment for optimized production of high content lignin-cellulose nanofibrils. Int J Biol Macromol 209:413–425. https://doi.org/10.1016/j.ijbiomac.2022.04.005
Ek M, Gellerstedt G (2009) Wood chemistry and biotechnology. Walter de Gruyter
Espinosa E, Tarrés Q, Delgado-Aguilar M et al (2016) Suitability of wheat straw semichemical pulp for the fabrication of lignocellulosic nanofibres and their application to papermaking slurries. Cellulose 23:837–852. https://doi.org/10.1007/s10570-015-0807-8
Espinosa E, Sánchez R, Otero R et al (2017) A comparative study of the suitability of different cereal straws for lignocellulose nanofibers isolation. Int J Biol Macromol 103:990–999. https://doi.org/10.1016/j.ijbiomac.2017.05.156
Fernández-Fernández M, Sanromán MA, Moldes D (2014) Potential of laccase for modification of Eucalyptus globulus wood: a XPS study. Wood Sci Technol 48:151–160. https://doi.org/10.1007/s00226-013-0593-0
Ferraz A (2000) Estimating the chemical composition of biodegraded pine and eucalyptus wood by DRIFT spectroscopy and multivariate analysis. Bioresour Technol 74:201–212. https://doi.org/10.1016/s0960-8524(00)00024-9
Filgueira D (2018) Biotechnology applied to the modification of lignocellulosic materials: improvement of the surface properties and manufacturing of biocomposites for 3D printing. Universidade de Vigo
Filgueira D, Holmen S, Melbø JK et al (2017) Enzymatic-assisted modification of thermomechanical pulp fibers to improve the interfacial adhesion with poly (lactic acid) for 3D printing. ACS Sustain Chem Eng 5:9338–9346
Ghose TK (1987) Measurement of cellulase activities. Pure Appl Chem 59:257–268. https://doi.org/10.1351/pac198759020257
Han X, Bi R, Khatri V et al (2021) Use of endoglucanase and accessory enzymes to facilitate mechanical pulp nanofibrillation. ACS Sustain Chem Eng 9:1406–1413. https://doi.org/10.1021/acssuschemeng.0c08588
Henríquez-Gallegos S, Albornoz-Palma G, Andrade A et al (2021) Impact of the enzyme charge on the production and morphological features of cellulose nanofibrils. Polymers (basel) 13:3238. https://doi.org/10.3390/polym13193238
Iglesias MC, Shivyari N, Norris A et al (2020) The effect of residual lignin on the rheological properties of cellulose nanofibril suspensions. J Wood Chem Technol 40:370–381. https://doi.org/10.1080/02773813.2020.1828472
Jiang C, Cao T, Wu W et al (2017) Novel approach to prepare ultrathin lignocellulosic film for monitoring enzymatic hydrolysis process by quartz crystal microbalance. ACS Sustain Chem Eng 5:3837–3844. https://doi.org/10.1021/acssuschemeng.6b02884
Jiang Y, Liu X, Yang Q et al (2018) Effects of residual lignin on mechanical defibrillation process of cellulosic fiber for producing lignocellulose nanofibrils. Cellulose 25:6479–6494. https://doi.org/10.1007/s10570-018-2042-6
Kumar L, Arantes V, Chandra R, Saddler J (2012) The lignin present in steam pretreated softwood binds enzymes and limits cellulose accessibility. Bioresour Technol 103:201–208. https://doi.org/10.1016/j.biortech.2011.09.091
Li Y, Fu Q, Rojas R et al (2017) Lignin-retaining transparent wood. Chemsuschem 10:3445–3451. https://doi.org/10.1002/cssc.201701089
Liu Y, Chen B, Lv Y et al (2022) Insight into the performance of lignin-containing cellulose nanofibers (LCNFs) via lignin content regulation by p-toluenesulfonic acid delignification. Cellulose 29:2273–2287. https://doi.org/10.1007/s10570-022-04432-w
Mansfield ML, Douglas JF (2008) Transport properties of wormlike chains with applications to double helical DNA and carbon nanotubes. Macromolecules 41:5412–5421. https://doi.org/10.1021/ma702837v
Moldes D, Vidal T (2012) Laccase for biobleaching of eucalypt kraft pulp by means of a modified industrial bleaching sequence. Biotechnol Prog 28:1225–1231. https://doi.org/10.1002/btpr.1594
Moldes D, Díaz M, Tzanov T, Vidal T (2008) Comparative study of the efficiency of synthetic and natural mediators in laccase-assisted bleaching of eucalyptus kraft pulp. Biores Technol 99:7959–7965
Mooney CA, Mansfield SD, Touhy MG, Saddler JN (1998) The effect of initial pore volume and lignin content on the enzymatic hydrolysis of softwoods. Bioresour Technol 64:113–119. https://doi.org/10.1016/s0960-8524(97)00181-8
Nakagame S, Chandra RP, Saddler JN (2011) The influence of lignin on the enzymatic hydrolysis of pretreated biomass substrates. In: ACS symposium series. American Chemical Society, Washington, DC, pp 145–167
Nlandu H, Belkacemi K, Chorfa N et al (2022) Laccase-mediated grafting of phenolic compounds onto lignocellulosic flax nanofibers. J Nat Fibers 19:222–231. https://doi.org/10.1080/15440478.2020.1738307
Rodríguez-Couto S (2019) Fungal Laccase: a versatile enzyme for biotechnological applications. In: Recent advancement in white biotechnology through fungi. Springer, Cham, pp 429–457
Roth S, Spiess AC (2015) Laccases for biorefinery applications: a critical review on challenges and perspectives. Bioprocess Biosyst Eng 38:2285–2313. https://doi.org/10.1007/s00449-015-1475-7
Rumble J (ed) (2023) CRC handbook of chemistry and physics, 104th edn. CRC Press, London
Saleem R, Khurshid M, Ahmed S (2018) Laccases, manganese peroxidases and xylanases used for the bio-bleaching of paper pulp: an environmental friendly approach. Protein Pept Lett 25:180–186. https://doi.org/10.2174/0929866525666180122100133
Sharma PR, Varma AJ (2014) Thermal stability of cellulose and their nanoparticles: effect of incremental increases in carboxyl and aldehyde groups. Carbohydr Polym 114:339–343. https://doi.org/10.1016/j.carbpol.2014.08.032
Tarrés Q, Saguer E, Pèlach MA et al (2016) The feasibility of incorporating cellulose micro/nanofibers in papermaking processes: the relevance of enzymatic hydrolysis. Cellulose 23:1433–1445. https://doi.org/10.1007/s10570-016-0889-y
Wan Z, Wang L, Ma L et al (2017) Controlled hydrophobic biosurface of bacterial cellulose nanofibers through self-assembly of natural Zein protein. ACS Biomater Sci Eng 3:1595–1604. https://doi.org/10.1021/acsbiomaterials.7b00116
Xu Y, Yang S, Zhao P, Wu M, Song X, Ragauskas AJ (2021) Effect of endoglucanase and high-pressure homogenization post-treatments on mechanically grinded cellulose nanofibrils and their film performance. Carbohyd Polym 253:117253
Ying W, Shi Z, Yang H et al (2018) Effect of alkaline lignin modification on cellulase–lignin interactions and enzymatic saccharification yield. Biotechnol Biofuels. https://doi.org/10.1186/s13068-018-1217-6
Yuan T, Zeng J, Wang B et al (2021) Lignin containing cellulose nanofibers (LCNFs): lignin content-morphology-rheology relationships. Carbohydr Polym 254:117441. https://doi.org/10.1016/j.carbpol.2020.117441
Zhou C, Wang Y (2020) Recent progress in the conversion of biomass wastes into functional materials for value-added applications. Sci Technol Adv Mater 21:787–804. https://doi.org/10.1080/14686996.2020.1848213
Acknowledgments
S. Henríquez-Gallegos thanks the Postgraduate Department of the University of Concepción for granting a scholarship for the development of his postgraduate studies. The ASIF laboratory (Department of Chemical Engineering, Universidad de Concepción, CHT Group Chile (Eng. Carlos Oliveros), and Novozymes Spain, S.A. (Account Manager Ramiro Martinez Gutierrez).
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This work was funded by the Innovation Fund for Competitiveness of the Chilean Economic Development Agency (CORFO) under Grant no. 13CEI2-21839.
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SH-G Conceptualization, Methodology, Validation, Formal analysis, Investigation, Writing—Original Draft. GA-P Formal analysis, Investigation, Writing—Original Draft, Review and Editing. AA Formal analysis. DM Methodology, Writing—Original Draft, Review and Editing. AM-M Formal analysis. RTM Writing—Review and Editing, Supervision. MP Conceptualization, Validation, Resources, Writing—Review and Editing, Supervision, Funding acquisition.
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Henríquez-Gallegos, S., Albornoz-Palma, G., Andrade, A. et al. Effect of enzyme lignin oxidation by laccase on the enzymatic-mechanical production process of lignocellulose nanofibrils from mechanical pulp. Cellulose 31, 3545–3560 (2024). https://doi.org/10.1007/s10570-024-05784-1
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DOI: https://doi.org/10.1007/s10570-024-05784-1