Isolation of Microcrystalline Cellulose (MCC) from Rice Husk: A Review

 

Sylma Dhini Avitra¹, David Fernando², Marlyn Dian Laksitorini¹,

Teuku Nanda Saifullah Sulaiman¹*

¹Department of Pharmaceutics, Faculty of Pharmacy, Universitas Gadjah Mada,

Daerah Istimewa Yogyakarta 55281, Indonesia.

²Department of Pharmaceutical Chemistry, Faculty of Pharmacy, Universitas Gadjah Mada,

Daerah Istimewa Yogyakarta 55281, Indonesia.

 

ABSTRACT:

 

 

INTRODUCTION: 

RH, as a by-product of the shelling process, accounts for about 20% of total rice weight¹. Despite its reputation as an environmental hazard², it is known to have critical nutritional values, including cellulose, hemicellulose, lignin, hydrated silica, organic carbons, and potassium^1,3–7. MCC is a naturally formed polymer that is made up of units of glucose linked to one another (see Figure 1).

 

 

Figure 1. Structure of Microcrystalline Cellulose

 

MCC is mainly made in four steps: delignification, bleaching, acid hydrolysis, and drying^8,9. The advancements in various production, modification, and advanced applications of both MCC and NCC were reviewed by Haldar and Purkait, 2020¹⁰. Another review, conducted by Belali et al., 2019¹¹, focused on the isolation of MCC and how it affects the post-compression properties of the material. However, neither the RH nor the optimization of the MCC separation method are highlighted in either Furthermore, Trache et al., 2016¹² covered the utilization of MCC in biocomposites as well as its characterization and separation. Apart from that, this review does not emphasize the improvement of MCC made with RH. The preparation and techniques used to characterize MCC for pharmaceutical excipients are also covered in a review by Cahyani et al., 2022⁸. Unlike the prior review, this review does not focus on the characterization and optimization of MCC's isolated from RH.

 

To the author's knowledge, no other reviews have addressed this subject, particularly the improvement of MCC isolation from RH. A wide range of circumstances influences the efficiency of these stages, and this subject has been the subject of extensive optimization research. An evaluation is crucial to ascertain the ideal conditions for extracting MCC from RH, particularly about the solvents or methodologies employed in each processing stage. This review aimed to emphasize the application of solvents and procedures in optimizing the production of MCC from RH. The features of MCC generated by various isolation techniques using RH (particularly %CrI)  are also examined in this research.

 

METHODS:

Several databases (Scopus, Google Scholar, and Pubmed) were used to extract potential articles. Boolean instructions were used to remove pointless journals from the search. (MCC or microcrystalline cellulose) AND “rice husk” AND isolation is included in the keyword search. After duplicates were removed, articles were rejected during each screening stage. There are 406 articles in all that have been collected that could be useful. Publications that focus on MCC isolation, provide data on the proportion of MCC yield, and were conducted within the last ten years (2013–2023) are included in this evaluation; other publications are disregarded. Following that, the articles are subjected to an abstract screening procedure before undergoing a second examination by two researchers. To be included, both researchers must approve an article; if one of them rejects it, a third party will be consulted. Eligible articles are also manually extracted using the snowballing process.

 

RESULTS AND DISCUSSION:

The stages of MCC’s isolation are associated with several essential responses, such as cellulose yield (% wt/wt), MCC yield (% wt/wt), and %CrI. Cellulose is typically acquired post-delignification, and MCC is generally derived via hydrolysis. CrI is employed to assess the degree of crystallinity in cellulose, indicating the proportion of crystalline vs amorphous cellulose in the sample¹³. Figure 2 provides a summary of each step's optimization parameter. Each phase and associated optimization parameter will be further highlighted.

 

Figure 2. Optimization of MCC Isolation from Rice Husk

 

Figure 3. MCC production from rice husk through delignification and hydrolysis process

 

Delignification:

The process of delignification is to separate lignocellulose into cellulose, hemicellulose, and lignin¹⁴. To optimize the process, lignin characteristics must be exploited during pre-treatment to produce pure cellulose. Phenylpropane molecules joined by many bonds to form a polymer with an aromatic structure is what makes up lignin^12,15. Figure 4 is an illustration of the lignin structure which physically encloses microfibrils in a hydrophobic matrix and is covalently bound to hemicellulose so as to prevent hydrolysis of the cellulose polymer.

 

Several pulping sequences and techniques can be used to achieve RH delignification in various situations, including chemical, mechanical, and biological pulping. Table 3 provides a summary of these strategies' benefits and drawbacks. This finding is consistent with Tables 1 and 3, which demonstrate that alkaline pulping (NaOH) is typically used to treat 100% of the delignification process. It is also customary to experiment with various steps of delignification, time used, temperature ranges, stirring speeds, and NaOH concentrations in order to determine the optimal delignification procedure. The delignification method is assumed to be more optimal when cellulose or MCC is achieved. According to Table 1, the best conditions for the delignification process are NaOH 1M at 80°C for 1.5 hours without stirring; this results in an overall MCC of 83.5% and a CrI of 52.4%. However, as the data sets contain a variety of optimization parameters, this result does not demonstrate that a particular parameter or the use of stirring correlates with the yield of MCC.

 

Table 1. Delignification stage of rice husk microcrystalline cellulose extraction

Label	ΣRH (g)	Delignification 1x or 2x				Washing	Bleaching	Hydrolysis	Drying	Yield Cellulose (%)	References
		Solvent	T (⁰C)	Duration	Stirring
A1	100	NaOH 10%	55	1.5 h	Yes	Yes	Yes	Yes	Yes	38.35	16
A2										36.14
A3										36.65
A4	10	NaOH 12%	80	3 h	Yes	Yes	Yes	No	No	52.3	17
A5	10	NaOH 1M	80	1.5 h	Yes	Yes	Yes	Yes	Yes	-	18
A6	400	NaOH 5%	120	0.75 h	No	Yes	No	Yes	Yes	-	19
A7										-
A8	400	NaOH 5%	120	0.75 h	No	Yes	Yes	No	Yes	68.96
A9	10	NaOH 1M	80	1.6 h	No	No	Yes	Yes	Yes	-	20
A10										-
A11										-
A12										-
A13	10	NaOH 1M	80	1.5 h	No	Yes	Yes	Yes	Yes	-	21
A14										-
A15										-
A16	200	NaOH 4M	80	24 h	Yes	No	Yes	Yes	Yes	-	22
A17	1500	NaOH 2%	100	3 h	No	No	Yes	No	Yes	33.33	23
		NaOH 17.5%	80	1 h	No	Yes
A18	450	NaOH 2%	100	3 h	No	No	Yes	Yes	Yes	-	24
		NaOH 17.5%	80	1 h	No	Yes
A19	350	NaOH 4%	80	2 h	No	Yes	Yes	No	Yes	15.2	25
		NaOH 17.5%	80	1 h	No	Yes
A20	350	HNO3 3%	90	2 h	No	Yes	No	Yes	Yes	-	25
		NaOH 2% and Na2SO3 2%	50	1 h	No	Yes	Yes
		NaOH 17.5%	80	0.5 h	No	Yes	Yes

Notes : Different labels represent samples that are treated in a different way according to the reference.

 

Table 2. The process of bleaching, hydrolysis, and drying of rice husk microcrystalline cellulose extraction

Label	Bleaching			Hydrolisis				Drying	Yield MCC (%)	CrI (%)	Ref.
	Solvent	T (⁰C)	Duration	Acid	T (⁰C)	Duration	Stirring
A1	NaClO2 0.5%	85	90 min	HCl 2.5N	105	20 min	Yes	Oven, 40⁰C at 20 h	25.05	-	16
A2	NaClO2 0.7%								23.25	-
A3	NaClO2 1.0%								22.75	64.74
A4	NaClO 2.5%	80	60 min	-	-	-	-	-	-	58.73	17
A5	NaClO 5%	80	18 min	HNO3 1M	80	30 min	Yes	Oven, 100⁰C constant weight	-	42	18
A6	-	-	-	H2SO4 5%, CH3COOH 25%, H2O2 5%	120	120 min	No	60⁰C at 24 h	63.38	72.88	19
A7				HNO3 10%, CH3COOH 25%, H2O2 5%	120	120 min	No	60⁰C at 24 h	65.51	79.29
A8	NaClO2 8g and CH3COOH  1.47%	70	300 min	-	-	-	-	60⁰C at 24 h	-	61.86
A9	NaClO 5%	80	18 min	HNO3 1M	25	30 min	Yes	Dried, Not specified	80.64	42.0	20
A10				HCl 1M					60.58	37.0
A11				HNO3 2M					83.26	63.9
A12				HCl 2M					69.24	52.2
A13	NaClO 5%	80	18 min	HNO3 0.5M	80	30 min	Yes	Oven, 70⁰C at 24 h	83.5	52.4	21
A14				H2SO4 0.5M					80.6	49.7
A15				HCl 0.5M					81.8	54.2
A16	NaClO 12.5%	40	60 min	H2SO4  98%	60	60 min	Yes	Oven, 40⁰C at 24 h	-	47.6	22
A17	NaClO 3.2%	40	120 min	-	-	-	-	Oven, 60⁰C at 16 h, sifted, 60⁰C at 1 h	-	-	23
A18	NaClO 3.2%	40	120 min	HCl 2.5N	100	30 min	No	60⁰C	17.11	-	24
A19	NaClO	40	40 min	-	-	-	-	60⁰C at 1 h	-	-	25
	NaClO	80	20 min
A20	NaClO 3.5%	Boiling	20 min	HCl 2.0 N	Boiling	15 min	Yes	Fluidized bed, 57-60⁰C at 1 h	11.7	50	25
	NaClO 1.75%	100	5 min

Notes : Different labels represent samples that are treated in a different way according to the reference.

 

Table 3. Comparison of Different Delignification Process^14,15,26,27

Type	Treatment	Pros	Cons
Chemical Pulping	Kraft/ Sulfate	Variety of wood usage, efficient usage and recovery of product, requires less time	High residual lignin, high energy usage, environmentally damaging, higher cost
	Neutral Sulfite	Brighter pulp that is easy to bleach, higher yield (8-10%) than alkaline pulping, less time required	Resinous softwoods, tannin-bearing hardwoods, and supplies containing bark are not tolerated, higher cost
	Acidic Sulfite	Overcome low lignin and hemicelluloses pulp, less time required	Emission of SO2 causes air pollution, higher cost
	Alkaline	Odorless gas (environmentally friendly), less time required, high efficiency	Higher cost
Mechanical Pulping	Size reduction, Temperature, Stirring and Pressure	Cheaper to produce (about half the cost of chemical pulping), Higher accessibility to matrix	High energy demand, weaker than chemical pulping, high lignin residual
Semi-Chemical Pulping	Mechanical and Chemical	Higher accessibility to matrix, high efficiency and less time required	High energy demand, high cost
Biological Pulping	Bacteria or fungi	Low cost and energy demand	Low efficiency and slower rate of lignin degradation (depends on microorganism used)

 

The amount of delignification operations is found to have a negative correlation with the MCC yield. Single-step delignification produces a higher overall percentage of MCC (63.17% and 17.11%, respectively) than two-step delignification processes (Figure 5). Frequent use of these compounds produce byproducts that impede cellulose hydrolysis even more, lowering the process's yield^28,29. It is impossible to determine a correlation between these factors and the yield percentage of cellulose, MCC, or CrI using the data set in Table 1. This is a result of the several studies that were conducted with varying sets of methods and report parameters (many of which are not reported based on Figure 5). More research is needed to discover how the solvent content, sample-to-solvent ratio, temperature, delignification time, and stirring technique affect the percentage yield of MCC, cellulose, and CrI from RH.

 

Bleaching:

In conjunction with delignification, bleaching processes use chemicals to increase the purity of cellulose³⁰ and dissolve lignin from fibrous materials³¹. Oxidators, such as hydrogen peroxide (H₂O₂), sodium hypochlorite (NaClO), sodium chlorite (NaClO₂), chlorine (Cl₂), and ozone (O₃) are frequently utilized in this bleaching process. The benefits and drawbacks of each bleaching chemical for enhancing pulp color are listed in Table 4. NaClO is the most commonly utilized (as seen in Table 2) in the bleaching process compared to NaClO₂ and H₂O₂. This is due to its ease of acquisition and application, as well as its comparatively lower cost.

 

Table 4. Comparison of Different Bleaching Reagents^26,32-34

Bleaching Phase	Bleaching Treatment	Molecular Formula	Pros	Cons
Liquid phase bleaching	Sodium Hypochlorite	NaClO	Cheaper than NaClO2, cost-effective, easy to obtain and use	Unstable solution, degrade under sunlight
	Sodium Chlorite / Chlorine Dioxide	NaClO2 / ClO2	Stable solution, longer shelf life	More expensive than NaClO, ClO2 released is environmentally damaging
	Hydrogen Peroxide	H2O2	Environmentally friendly, Surface friendly and widely used for dental bleaching	Less aggressive (Compared to NaClO, and NaClO2), Less favorable in bleaching wood/ porous materials
Gas phase bleaching	Chlorine	Cl2	Low cost (Compared to O3)	Environmentally damaging to ozone layer
	Ozone	O3	Environmentally friendly, Faster and stronger oxidation (Compared to Cl2)	High cost (Compared to Cl2), Complicated equipment setups

 

Lower levels of biochemical and chemical oxygen demand, color, adsorbable organic halides, and the formation of chlorophenolic compounds have been found when ozone is added, followed by ClO₂ and hydrogen peroxide³⁵. Table 2, however, illustrates that gas phase bleaching is not commonly utilized in laboratory settings for the purpose of whitening RH. This might be caused by the difficult standard conditions (such as the temperature and pressure), the high cost, the advanced materials, and the difficult equipment setup that must be completed in the laboratory. Surprisingly, the unbleached samples (Figure 4) have the highest %CrI, suggesting that the bleaching procedure has a negative correlation with the rise of %CrI of the samples.

 

Figure 4. Output visualization of %Cellulose, %MCC, and %CrI from various treatment (A1-A20 represent the data label obtained from Table 2 & 3, while any unavailable data were represented as 0)

 

These results also agree with those of Gümüşkaya (2002), who found that lignin removal using bleaching techniques might lead to an increase in the %CrI³⁶. When comparing unbleached to bleached Eucalyptus pulps, higher intensity of X-ray diffraction patterns is also seen³⁷, further indicating that the bleaching process may have a major influence on reducing the %CrI of RH. Meanwhile, it is impossible to draw conclusions about the link between different bleaching chemicals, concentration, temperature, and duration to %cellulose and %MCC. This is because the independent variables in the research that was included in this study are not evenly controlled, which leads to their unpredictability. Further research is required to conclude if these parameters have an impact on the yield of cellulose, MCC, and CrI.

 

Hydrolysis:

Various methods can be employed to extract and purify MCC, such as enzymatic hydrolysis^38,39, acid hydrolysis^40-42, and steam explosion⁴³. Enzymatic hydrolysis yields a higher purity of MCC in comparison to acid hydrolysis. Nevertheless, the process of breaking down enzymes like cellulase is associated with significant expenses and limited effectiveness in the MCC synthesis⁴⁴. The acid hydrolysis procedure is preferred over others because of its shorter time. In this degradation condition, the yield produced by H₂SO₄ could be less than HCl. This can be seen in Table 2 (A13-A15) which reported that the lowest yield of hydrolysis results was using H₂SO₄ compared to HCl and HNO₃. HCl and H₂SO₄ are extremely corrosive^45,46, so their utilization is taken into consideration during the development of MCC extraction. Alternatively, other weaker acids can be utilized, such as nitric acid.

 

HNO₃ is a strong acid that is slightly weaker than HCl and H₂SO₄ based on its pKa value⁴⁷. However, HNO₃ is able to hydrolyze lignocellulose with lower cellulose degradation than HCl and H₂SO₄. This is proven by the fact that HNO₃ preserves higher cellulose or MCC in several studies^19-21. Studies using HNO₃ for this process generate larger yields of %MCC (A9, A11, and A13) than other studies, as shown in Table 3 and Figure 5. In contrast, the majority of research with the lowest %MCC uses HCl to carry out the hydrolysis process (A1, A2, A3, and A18). The oxidative capacity of nitric acid, as opposed to HCl, likely facilitates the conversion of nitriles into carboxylic acids, hence increasing the yield of MCC from RH²¹. No research using phosphoric and citric acids to extract MCC from RH has come to our attention. Although phosphoric and citric acids haven't been employed as frequently as the previous acids to create MCC, they have been combined with strong acids to create Nanocrystalline Cellulose (NCC)^48,49. More research needs to be done to determine whether employing these acids is feasible and cost-effective.

 

Table 5. Comparison of Different Hydrolysis Treatments^21,44,50-53

Type of Treatment	Hydrolysis Treatment	Molecular Formula	Pros	Cons
Acid Treatment	Sulfuric Acid	H2SO4	Cost-effective, most effective acid hydrolysis agent	Extremely corrosive and hazardous, high energy usage,  high sugar yield
	Hydrochloric Acid	HCl	Less aggressive, lower sugar yield, corrosive and hazardous than H2SO4	Lower efficiency and reaction time
	Nitric Acid	HNO3	Produces the highest yield compared to H2SO4 and HCl	Hazardous and high energy usage, not suitable in glucose production, more expensive compared to H2SO4 and HCl
Enzymatic Treatment	Cellulase		Eco-friendly, high specificity, high efficiency, high purity MCC output	Expensive, not effective, slow reaction rate
Combined Treatment	Cellulase and Acid Treatment		High specificity, high efficiency, high purity output	Expensive
Steam Explosion / Autohydrolysis	High pressure and temperature		Applicable to various starting  materials, high efficiency	Not applicable as a pretreatment for acid hydrolysis, high energy usage

 

Drying:

It has been demonstrated that the drying process significantly affects the MCC's porosity, morphology, form, aggregation, and CrI^54,55. In order to create dry solids, the process of drying involves eliminating water and other liquids. Increasing or maintaining the material's qualities (such as its flowability) and material preservation are some of the process' goals^56,57. Some technologies that can be used are spray drying⁵⁸, freeze-drying/lyophilization, fluidized bed drying⁵⁴, microwave-aided drying⁵⁹, and oven drying¹⁶. Microwaves and ovens are the least expensive of the aforementioned solutions^57-59.

 

Acid hydrolysis is not necessary when drying using microwaves during the delignification and bleaching processes. According to the findings of FTIR and XRD examinations, this is because amorphous non-cellulose chemicals have been eliminated⁵⁹. However, this method has a drawback; namely, it is not easy to set the right temperature in its optimization⁶⁰. This is evidenced by the absence of significant differences in particle size and CrI in three different temperature settings in the microwave method⁶¹. In addition, the oven method is the least expensive on a small scale when compared to other drying techniques. On a laboratory scale, this approach is frequently utilized to dry MCCs despite its lengthy duration. This is due to the fact that, in addition to its cost, it is the simplest to operate when compared to other drying techniques⁵⁷. Table 3 illustrates this pattern as well. In this table, oven drying is used for the majority of the experimental processes, with temperature ranges of 40°C to 100°C and durations ranging from 1 to 24 hours.

 

The yield of MCC and cellulose is unaffected when the drying process alters the CrI, per theory. However, if the drying procedure is not adjusted, the water content may increase the MCC or cellulose yield unintentionally. Cellulosic fibers shrink during the drying process, which results in semi-irreversible pore closure and decreased fiber performance⁶². Because there are fewer amorphous patches as a result of this pore collapse, CrI is enhanced. A higher increase in the CrI is typically the result of more rigorous drying techniques. Products that are spray-dried, for instance, have more CrI than those that are not^63,64. The data collected (Table 3 and Figure 5) do not display this pattern; in fact, it was not discovered that the CrI of the undried (or rather, that information was not available for A4) samples was lower than that of the dried ones. This is explained by the fact that the experiment ended at the bleaching stage, indicating that when discussing CrI, the bleaching stage is more important than the drying stage. Based on the currently available data, further research is necessary to accurately evaluate the impact of the drying process (temperature, duration, and method) on CrI.

 

CONCLUSION:

RH is one of the materials that has the potential to be isolated into MCC through delignification, bleaching, acid hydrolysis, and drying processes. To achieve the highest possible MCC, optimizing many factors at each stage of the process is necessary. The delignification method yielded the maximum percentage of MCC (83.5%) and a CrI of 52.4% while using a 1M NaOH solution at 80°C for 1.5 hours without stirring. Furthermore, it was shown that an increase in the number of delignification repetitions decreased the %MCC production. During the acid hydrolysis process, it was noted that HNO₃ is preferable due to its ability to generate a substantial amount of cellulose and MCC yield. The final step, drying, impacts the physical properties of MCC. Although bleaching reduces the %CrI of samples, further study is needed because it is impossible to infer a relationship between the amount of cellulose and MCC and the various bleaching chemicals, concentrations, temperatures, and bleaching treatment times. This is because different research backgrounds were used to collect the independent variables, resulting in uneven control over them.

 

ABBREVIATIONS:

Cl₂          = Chlorine

CrI          = Crystallinity Index

H₂O₂      = Hydrogen Peroxide

MCC      = Microcrystalline Cellulose

RH          = Rice Husk

NaClO₂  = Sodium Chlorite

NaClO    = Sodium Hypochlorite

O₃           = Ozone

 

ACKNOWLEDGEMENTS:

We especially acknowledge the Indonesia Endowment Fund for Education Agency (LPDP) from the Ministry of Finance of the Republic of Indonesia for supporting the publication of this paper.

 

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Received on 09.09.2024      Revised on 21.01.2025 Accepted on 12.04.2025      Published on 02.08.2025 Available online from August 08, 2025 Research J. Pharmacy and Technology. 2025;18(8):3979-3986. DOI: 10.52711/0974-360X.2025.00572 © RJPT All right reserved
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