Production of nanocrystalline cellulose from bleached soda bagasse pulp

Ashrafi Birgani, S., Talaeipour, M., Hemmasi, A. H., Bazyar, B., and Larijani, K. (2021). "Production of nanocrystalline cellulose from bleached soda bagasse pulp," BioResources 16(4), 7817-7829.

Abstract

The cellulose used in this study was prepared from bleached soda bagasse obtained from the Pars paper factory. To prepare nanocellulose, the sample was subjected to alkaline pretreatment and then acid hydrolysis using 54% sulfuric acid at several temperatures (35, 50, 60, and 65 °C) and different times (30, 60, 90, and 120 min). Then, they were prepared using a centrifuge, dialysis bag, ultrasound, and freezer, respectively. The produced nanocellulose was characterized by transmission electron microscopy (TEM), field-emission scanning electron microscopy (FE-SEM), Fourier transform infrared spectroscopy (FTIR), and X-ray diffraction (XRD). According to the results, temperatures of 50 and 90 °C were selected for the preparation of nanocellulose. The crystallization index of the hydrolyzed pulp and produced nanocellulose was 53 and 61%, respectively. The produced nanocellulose had a fibrillar shape.

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Production of Nanocrystalline Cellulose from Bleached Soda Bagasse Pulp

Sabah Ashrafi Birgani,^a Mohammad Talaeipour,^a,* Amir Hooman Hemmasi,^aBehzad Bazyar,^a and Kambiz Larijani ^b

Keywords: Nanocrystalline cellulose; Bagasse; Acid hydrolysis; Nano technology

Contact information: a: Department of Wood and Paper Science and Technology, Faculty of Natural Resources and Environment, Science and Research Branch, Islamic Azad University, P. O, Box 14515/775, Tehran, Iran; b: Department of Chemistry Science and Research Branch, Islamic Azad University, Tehran, Iran; P. O, Box 14515/775; *Corresponding author: m.talaeipoor@srbiau.ac.ir

INTRODUCTION

Cellulose is the most abundant polymeric raw material found in nature (Henriksson and Berglund 2007; O’Connell et al. 2008; Gama et al. 2012; Faruk et al. 2012; Vazquez et al. 2015; Zhu et al. 2016; Trache et al. 2016a,b; Santos et al. 2017; Ribeiro et al. 2019); 10¹⁰ to 10¹²tons are produced annually (Postek et al. 2013). Only a small part of it (10⁹ × 6 tons) is used in various industrial fields for example, paper, textile, industries, and chemistry (Trache et al. 2020 a, b). In general, cellulose is a fibrous, water-insoluble, strong substance that plays a key role in maintaining the structure of plant cell walls (Habibi et al. 2010). The properties of cellulosic fibers are greatly influenced by factors such as their internal fiber structure, microfibril angle, chemical composition, and cell dimensions, which vary between parts of the same plant and between plant species (Siqueira et al. 2010). Ignoring its source, Cellulose is a linear polysaccharide with D-glucopyranose bond joined by β-1,4 glycoside bonds (Henriksson and Berglund 2007; O’Connell et al. 2008; Faruk et al. 2012) (Fig. 1). There are three hydroxyl groups in cellulose. The primary hydroxyl is in the methylol group (-CH₂OH) at C-6, and there are secondary hydroxyl groups (-OH) on C-3 and C-4. Each monomer unit rotates 180° relative to its adjacent monomers. Though it is a linear polysaccharide containing hydrophilic hydroxyl groups, it does not dissolve in water and common solvents due to the multiplicity of hydrogen bonds between the cellulose chains. A combination of hydrogen bonds between cellulose chains and van der Waals forces between glucose units lead to the formation of crystalline regions in cellulose (O’Connell et al. 2008). The cell wall of wood cells is formed by the accumulation of cellulose, lignin, and hemicellulose. Cellulose fibers bind to each other with the help of lignin, and hemicellulose acts as a binder between cellulose and lignin. The number of hydrogen bonds plays an important role in the formation of cellulose and cellulose fibers.

Fig. 1. The structure of cellulose

Cellulose structure is composed of two parts: crystalline and amorphous. The amorphous region is the most susceptible for an acid or enzyme hydrolysis (Dufresne 2013; Kargarzadeh et al. 2017; Tarchoun et al. 2019a, b, c; Ribeiro et al. 2019). Cellulose can be obtained from a variety of sources, such as wood, herbaceous plants, grass, agricultural products and by-products, animal sources, algae, and bacteria (Trache et al. 2017; Nandi and Guha 2018; Kumar et al. 2020). Cellulose is a natural, biodegradable, environmentally friendly, and renewable material that has different physical, chemical, optical, magnetic, and biological properties due to its constituent raw materials (Jin et al. 2014; He et al. 2019). Cellulose crystals, nanocrystals, viscose, nanofibrils, and nanofibers have been produced (Siro and Plackett 2010). The properties of nanocelluloses including surface-to-volume ratio (high specific surface area), high modulus and tensile strength, low thermal expansion weakness, high hydrogen bonding capacity, biodegradability, high specific surface area, high rigidity, and non-toxicity (Siro and Placket 2010; Habibi et al. 2010; Moon et al. 2011; Klemm et al. 2011; lavoine 2012; Zhou et al. 2014; Salimi et al. 2019 ) have made this unique nanomaterial useful for research (Foster et al. 2018; Salimi et al. 2019). This provides the basis for its entry into more advanced applications (Yassin et al. 2019). In general, nanocellulose is classified into two main groups: nanofibers (bacterial cellulose, cellulose nanofibrils and cellulose nanocrystals) and nanostructured materials (including nanofibrillated cellulose and microfibrillated cellulose) (Trache et al. 2017; Hussin et al. 2019; Pennells et al. 2020). Different forms of nanocelluloses can be prepared using different methods and from various cellulosic sources (Phanthong et al. 2018; Pires et al. 2019; Salimi et al. 2019).

Characteristics of each nanocellulose class such as size and morphology depend on the processing conditions, the isolation, and cellulose origin. (Li et al. 2018; Vilarinho et al. 2018; Pires et al. 2019; Köse et al. 2020). The preparation of nanocellulose usually requires two steps (Trache et al. 2017; Nandi and Guha 2018; Xie et al. 2018). In the first stage, the extracted materials (monomers, dimers, and lipid polymers, sugars, tannins, resins, flavonoids, terpenoids, terpenes, waxes, fatty acids, etc.), hemicelluloses, and lignin are partially or completely eliminated from the source by special pretreatment methods (Taipina 2012; Kargarzadeh et al. 2017). Second, the removal of amorphous regions of crude cellulose results in production of cellulose nanocrystal (CNC) (Dufresne 2013). After the second step, other treatments, such as solvent removal, neutralization, washing, purification, centrifugation, ultrasound, dialysis, stabilization, and drying (freezing and spray drying) can be performed (Lavoine et al. 2012; Taipina 2012; Trache et al. 2020). The most common process for producing nanocrystals uses strong acids such as hydrochloric acid, which produce highly crystalline nanoparticles (Klemm et al. 2018). An example of nanocellulose production from hardwood is shown in Fig. 2. Although production of nanocellulose from various natural sources has been extensively studied, the use of the bleached soda bagasse pulp as a source of natural fiber has not been investigated fully. Bagasse is a by-product of the sugarcane factories. Sugarcane bagasse contains about 40 to 50% cellulose in its composition, much of which is in the crystalline structure (Wulandari et al. 2016). Due to its characteristics such as availability, low lignin content, and low cost, it is a promising raw material for extraction and production of nanocellulose. This study extracted CNC from bleached soda bagasse pulp using alkaline pretreatment followed by acid hydrolysis (H₂SO₄).

Fig. 2. An example of CNC production steps from hardwood (Lin et al. 2019)

EXPERIMENTAL

Materials

Bleached soda bagasse pulp was prepared from the Pars Company. Chemicals such as potassium hydroxide, acetic acid, sodium hydroxide, and sulfuric acid were purchased from Merck (Darmstadt, Germany). The sample was subjected to alkaline hydrolysis and acid hydrolysis, followed by the other treatments including solvent removal, washing, purification, ﬁltration, centrifugation, dialysis, sonication, and freeze-drying.

Alkaline Hydrolysis (Production of Alpha Cellulose)

For removing pigments and producing alpha cellulose, 20 g of the bleached soda bagasse pulp was mixed with 8% caustic soda in a ratio of 20: 1 (relative to dry weight to acid) by a constant mixer for 90 min at 30 °C. The pulp was drained and washed with 100 mL of 2% potassium hydroxide, 200 mL of hot distilled water, 200 mL of acetic acid, and 2000 mL of cold distilled water.

Preparation of Nanocellulose

Alpha cellulose produced using 54% sulfuric acid was hydrolyzed at a 13:1 ratio. Cellulose hydrolysis was performed at several temperatures (35, 50, and 65 °C) and times (30, 60, 90, and 120 min). The reaction was stopped by adding 10 times distilled water (250 mL) to the solution. The suspension was centrifuged at 6500 rpm for 30 min and then placed in a dialysis bag for one week to neutralize and reach a pH level of 5. Neutral suspension was exposed to ultrasound for 10 min to produce homogeneous nanocellulose, which was then freeze-dried.

Scanning Electron Microscope (FE-SEM)

A TESCSN VEGAII model (Czech Republic) was operated with a voltage of 15 kW. For this purpose, a sample of carrier powders was placed on a carbon plate and was coated with gold with a thickness of 2 to 3 nm for 4 min.

Transmission Electron Microscope (TEM)

The dimensions of nanocelluloses were measured on a Zeiss-EM10C-100 KV TEM (Germany) with a voltage of 100 KW. For preparing the sample, the nanocellulose suspension was mildly ultrasonicated in a water bath for 10 min, and 1 mL of the solution was dropped on a grid. After a few min, the sample was ready for imaging.

Fourier Transform Infrared (FT-IR) Spectroscopy and Identification of Functional Groups

The FTIR analysis was performed using a Perkin Elmer RXI spectrometer (USA) at room temperature. The freeze-dried samples were mixed with KBr) Ratio 1 to 1000 mg) and pressed into tablets. The sample was scanned in a spectral range of 400 to 4000 cm^-1.

X-Ray Diffraction (XRD) Spectroscopy

X-ray diffraction patterns were recorded by Philips MPD X-ray generator (Netherlands) at 40 kV and 30 mA with X-ray radiation of  in the 2θ range of 5 to 50° with a scan step of 0.05°. The crystallinity index (CrI) was determined by the peak-height method (Segal et al. 1959) using Eq. 1,

CrI=[(I₀₀₂–I_am°)/I₀₀₂] ×100 (1)

where I₀₀₂ is the maximum diffraction intensity corresponding to 2θ (about 22) related to crystalline regions, and I_am is the minimum diffraction intensity at 2θ (about 18) related to amorphous region.

RESULTS AND DISCUSSION

Stability of the Suspension

The samples were studied for stability of the prepared suspensions. As shown in Fig. 3, all treatments were precipitated at 35 °C. One of the treatments was precipitated at 50 °C (30 min) after 5 min, indicating that these suspensions were in micro dimensions, while other suspensions remained stable until the end of the first week of the test.

Fig. 3. Images obtained by digital camera regarding suspension stability. Treatments at (a) 35 °C, (b) 50 °C, and (c) 65 °C

The stability of nanofiber suspensions is attributed to factors such as high specific surface area of nanofibers and high irregular and random movement of nanofibers in excess volume. During acid hydrolysis, temperature is a very important factor influencing acid activity. For example, at low temperatures (35 °C), mild acid activity occurs on cellulose chains. At the right temperature and time, the acid destroys amorphous regions of the cellulose chains, which are removed, causing formation of more crystals in the cellulose chains, as well as greater stability of the suspension. To select a treatment with stable suspension to produce nanocellulose, FE-SEM and FTIR analyses were performed.

Scanning Electron Microscope

In order to evaluate the size of nanocellulose produced in different samples and select the optimal conditions, electron microscopy was used. The FESEM images are shown in Fig. 2. The average length of nanocellulose was equal to 21.31, 13.82, 16.58, 17.64, 17.65, and 19.11 nm for the treatments studied under following conditions: 50 °C and 60 min, 50 °C and 90 min, 50 °C and 120 min, 30 °C and 65 min, 60 °C and 65 min, 90 °C and 65 min, and 120 °C and 65 min, respectively. The results showed that the sample obtained from 50 °C and 90 min were the smallest size.

Transmission Electron Microscope (TEM)

The TEM micrograph showed a very dilute suspension of nanocellulose from bleached soda bagasse. As shown in Fig. 4, nanocellulose particles accumulated in some places, while they were dispersed in the others. The particles were of fibrillar shape.

FT-IR Spectroscopy and Identification of Functional Groups

The FTIR spectra of different treatments are shown in Figs. 5 and 6. All samples exhibited a wide band in the range of 3200 to 3500 cm^-1, which is due to stretching vibration of O-H from OH groups of cellulose molecules (Khalil et al. 2001; Xu et al. 2005; Sain et al. 2006; Viera et al. 2007; Mandal and Chakrabarty 2011; Li et al. 2012; Lu and Hsieh 2012; Hokkanen et al. 2013; Rosli et al. 2013; Maiti et al. 2013; Kumar et al. 2014; Maryana et al. 2014; Li et al. 2014; Saelee et al. 2016; Almasian et al. 2016; Wulandari et al. 2016; Lam et al. 2017). The peak at 2894 cm^-1 is attributed to stretching modes of C-H in methyl and methylene functional groups, representing the main functional groups of cellulose (Mandal and Chakrabarty 2011; Lam et al. 2017). This range was not observed for samples with temperature and time conditions of 65 °C and 60, 90, and 120 min, but it was observed for the other samples. The peak from 1649 to 1641 cm^-1 was also related to O-H vibration of the adsorbed water (Ramo et al. 2000; Alemdar and Sain 2008; Mandal and Chakrabarty 2011; Li et al. 2012; Hokkanen et al. 2013; Almasian et al. 2016; Wulandari et al. 2016). The peak at 1250 cm^-1 represents aryl groups in lignin, found only in the bleached soda bagasse pulp sample, but it was decreased in the other samples. The peak from 890 to 820 cm^-1 is related to the vibration of COS and CS bond (Wei et al. 2014; Niu et al. 2017).

The results showed that carboxyl groups and sulfate esters were present in all samples. The slight increase of the adsorbing band at 1108 to 1100 cm^-1, attributed to sulfate, supported the possibility of sulfate ester formation (Wei et al. 2014). Moreover, one peak at 894 cm^-1 is attributed to glycoside CH deformation by ring vibration and O-H bending, which is related to b-glycoside bonds between anhydro-glucose units in cellulose (Nelson and O’Connor 1964; Alemdar and Sain 2008; Mandal and Chakrabarty 2011; Wulandari et al. 2016). This peak was seen only in the bleached soda bagasse pulp sample.

Fig. 4. Images obtained by FE-SEM of produce nanocellulose for different temperatures and time period at (A) 50 °C and 60 min, (B) 50 °C and 90 min, (C) 50 °C and 120 min, (D) 65 °C and 30 min, (E) 65 °C and 60 min, (F) 65 °C and 90 min, (G) 65 °C and 120 min, and (H) TEM image of the produced nanocelluloses at 50 ˚C and 90 min

The peak intensity was decreased to 894 cm^-1 by increasing hydrolysis time, indicating that the glycosidic bond had been broken and more OH groups had been released (Niu et al. 2017). The peak at 1054 cm^-1 associated with tensile vibration of C-O-C bond and glycoside bridge (Mandal and Chakrabarty 2011) was observed only in the bleached soda bagasse pulp due to hydrolysis and gradual reduction of molecular weight in the other samples. The band at 1730 cm^-1 was related to C=O stretching vibration for ester and acetyl linkage in hemicellulose or lignin (Nelson and O’Connor 1964; Alemdar and Sain 2008; Mandal and Chakrabarty 2011; Li et al. 2014; Wulandari et al. 2016; Lam et al. 2017). The peaks from 1602 to 1604 and 1505 to 1511 cm^-1 are attributed to C=C stretching vibration of aromatic ring in lignin (Kumar et al. 2014), and tension is related to the band at 1245 cm^-1 resulting from C-O stretching vibration of aryl group in lignin (Mandal and Chakrabarty 2011; Rosli et al. 2013; Saelee et al. 2016). None of these groups were found in the FTIR spectrum of the studied cellulose fibers, confirming the removal of lignin. According to the results of FE-SEM and FTIR, a sample studied at 50 °C and 90 min was selected to determine crystallinity and capture TEM images.

Fig. 5. FTIR spectra of the bleached soda bagasse pulp and alkaline hydrolysis-subjected pulp, and acid hydrolysis-subjected pulp at 50 ˚C and 30 min, 60 min, 90 min and 120 min

Fig. 6. FTIR spectra bleached soda bagasse pulp and alkaline hydrolysis-subjected pulp

X-ray Diffraction Spectroscopy

XRD microscopic images of the hydrolyzed pulp and produced nanocellulose are shown in Fig. 7. With the increase in amount of non-cellulosic polysaccharides and dissolution of amorphous regions, more orientation occurs along a specific axis (Mandal and Chakrabarty 2011). Both diffraction diagrams showed two well-defined peaks at Ø₂=18 and Ø₂=22. Diffraction pattern related to the hydrolyzed pulp and produced nanocellulose was almost identical and similar to previous results (Mandal and Chakrabarty 2011; Guilherme et al. 2015; Wulandari et al. 2016; Niu et al. 2017). The crystallization index of the hydrolyzed pulp and produced nanocellulose was obtained as 53% and 61%, respectively. The increased degree of crystallinity was attributed to removal of hemicelluloses and lignin.

Fig. 7. XRD diagram of the hydrolyzed pulp (a) and produced nanocellulose (b)

CONCLUSIONS

The crystallization index of the hydrolyzed pulp and produced nanocellulose was 53% and 67%, respectively. The increased crystallinity is attributed to the removal of hemicelluloses and lignin. Relatively high crystalline degree of nanocellulose produced from bagasse makes it very promising in new industrial applications, for example, as a reinforcer in matrix of polymers produced by various industries.
Based on the results of TEM analysis, nanocellulose had a fibrillar shape. Nanocellulose particles accumulated in some places but were dispersed in others.
FTIR analysis showed the absence of bands in the ranges of 1725 to 1730 cm^-1, 1602 to 1604 cm^-1, and 1511 to 1505 cm^-1, indicating the removal of lignin and hemicellulose from the suspension.
At higher temperatures and at right time, the acid destroys amorphous regions of the cellulose chains. Destruction and removal of these regions causes crystallization of the cellulose chains as well as stability of the suspension.

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Article submitted: May 19, 2021; Peer review completed: June 20, 2021; Revised version received and accepted: Sept. 27, 2021; Published: October 6, 2021.

DOI: 10.15376/biores.16.4.7817-7829