The characteristics of corn gluten-free cookies with modified cellulose as food additives

Several investigations were conducted to enhance the properties of gluten-free bakery items. Challenges in the development of gluten-free products involve a reduction in development capacity and product texture. One potential solution is to enhance the quality of gluten-free products by incorporating food additives from modified cellulose. The objective of this research to formulate and assess the impact of incorporating modified cellulose (CMC, MC, HPMC, and MCG) on the characteristics of gluten-free cookies made from corn flour. The study employed a completely randomized design for its investigation. The factor used was the type of cellulose derivative with an additional concentration of 1% with two replications. Based on the results of the study, it was shown that the addition of types of cellulose derivatives affected the characteristics of colour, proximate analysis results, and texture of gluten-free cookies from corn flour. The development ratio of HPMC cookies was nominally the highest at 12.38 (mm/gram), although statistically there was no significant difference between treatments. The fat content of the control cookies was higher at 19.16% compared to other cookies with added cellulose derivatives. The carbohydrate content of HPMC cookies is the highest at 88.00% compared to other cookies. This resulted in the lowest energy value of HPMC cookies at 389.26 kcal compared to other cookies. The microstructural profile based on SEM (Scanning Electron Microscope) of the resulting cookies shows different porosity. Based on the research results, adding several cellulose derivatives can improve the characteristics of gluten-free cookies from corn flour.


Introduction
The surge in research initiatives on gluten-free products is in tandem with the rise in cases of celiac disease and gluten allergies.Celiac disease, also known as gluten enteropathy (GE), affects nearly 1% of the general population [1,2].The technology for processing gluten-free products involves the use of raw materials devoid of gluten-containing flour.Local flours have been identified and characterized by Herawati and Kamsiati [3].Non-gluten flour sources include various grains, nuts, seeds, and tubers [4,5].1309 (2024) 012005 IOP Publishing doi:10.1088/1755-1315/1309/1/012005 2 Protein-rich local flours like corn flour, rice flour, hanjeli flour, among others, serve as promising raw material sources for the production of bakery items.Naseer et al. [6] conducted a study focusing on the creation of gluten-free cookies using rice flour.They explored various modifications and formulations to ensure the consumer acceptance of dry bakery products [7,8,9].Cookies, characterized by a fundamental formula comprising flour, fat, and sugar, necessitate affordability, pleasing taste, desirable texture, and overall consumer acceptance throughout the commercialization phase [10].
A notable drawback of gluten-free products is their challenging expansion and distinct characteristics compared to bakery items produced from wheat flour.Gluten-free formulations often display reduced mechanical properties, texture formation, volume, crumb structure, shelf life, textural strength, and sensory attributes, thereby affecting the overall quality and acceptability of the final product [11,12].In the technology of gluten-free production processes, hydrocolloids can contribute to enhancing viscoelasticity, thereby improving product characteristics in the absence of gluten components [13].
Enhancing the qualities of bakery products can be achieved by incorporating hydrocolloid food additives.Certain hydrocolloid additives, classified as food additives, contribute to increased dough viscosity and enhanced texture during the proofing and baking stages of bakery product preparation [14].A potential hydrocolloid component is derived from abundantly available cellulose sources with an annual production capacity ranging from 1011 to 1012 tons [15].Various materials, including sugar cane bagasse, sorghum straw, cotton, wood, palm fruit bunches, and date palm fronds, serve as cellulose sources [16,17,18].Numerous wood species, containing approximately 45-50% cellulose, are commonly employed as the primary industrial raw materials for cellulose production.
Cellulose has the versatility to undergo various modifications, resulting in derivative products like CMC (Carboxymethyl Cellulose), which holds utility in both food and non-food applications [19].Modified cellulose additives, including CMC (Carboxymethyl Cellulose), MC (Methyl Cellulose), HPMC (Hydroxypropyl Methyl Cellulose), and MCG (Microcrystalline Cellulose Gum), are included in some food formulations.Hydrocolloid components suitable for bakery products encompass HPMC (Hydroxy Propyl Methyl Cellulose) and CMC (Carboxy Methyl Cellulose) [20], utilizing corn starch as a raw material.Cellulose derivatives like CMC, HPMC, and MC (Methyl Cellulose) incorporate hydrophilic and hydrophobic components, contributing to dough structure during the proofing process and forming networks during baking [14].
To improve the characteristics of cookies from corn flour, hydrocolloid components from cellulose derivatives can be added.Determining the effect of types of cellulose derivatives on the quality of gluten-free cookies is needed.In this research activity, modifications were made to the effect of adding types of cellulose derivatives to gluten-free corn cookies and to characterize the resulting products.

Material
The necessary materials for this research include Mugo commercial corn flour sourced from North Jakarta.Additionally, various chemicals are required, such as CMC Teknik from Setia Guna Bogor, and other cellulose derivatives (MC, HPMC, and GMC) from PT. Redo Jakarta.Reagents for chemical analysis will be procured from commercial suppliers.The essential equipment for the research comprises a mixer, oven, cookie cutters, Soxhlet, kjedahl, burette, scales, and a Minolta chromameter.

Method
During the initial phase, cookies were prepared using corn flour as the control.Subsequently, in the following phase, cookies were processed using corn flour with the addition of modified cellulose derivatives.The primary components employed in this research included corn flour, granulated sugar, refined sugar, egg whites, and food additives in the form of cellulose derivatives (CMC, HPMC, MC, MCG) at a concentration of 1%.
The processing steps encompass the blending of egg yolks with fine sugar until achieving homogeneity and expansion of the egg whites.Subsequently, all remaining dry ingredients are incorporated into the mixture of powdered sugar and egg whites until thoroughly blended.The entire dough is then shaped and subjected to baking in an oven at 150°C for a duration of 15 minutes until it reaches a cooked and dry state.The physicochemical attributes of the cookies were evaluated, covering parameters such as the swelling ratio (thickness/weight), swelling ratio (diameter/weight), colour (L,a,b, Hue), proximate analysis [21], organoleptic assessment, texture, and microstructure profiling utilizing the SEM tool as per the modification by Herawati et al [22].All collected data underwent compilation and subsequent analysis through ANOVA and Duncan's post hoc test using SPSS 24 software.

Colour Analysis
For colour analysis, the Chromameter CR 410 from Konica Minolta INC. was utilized to measure parameters such as Lightness (L), redness (a), and yellowness (b).The colour measurement procedure followed the methods outlined by Muhamad et al [23] and Selimovic et al [24].Before measurement, the instrument underwent a calibration process using black and white standards.During the analysis, the sample was positioned in a sample holder, covering the entire Chroma Meter lens.The values of L, a, and b were identified, where L represents whiteness or blackness, a denotes redness or greenness, and b signifies yellowness or blueness.The degree of whiteness, redness, and yellowness was calculated using the respective formulas as indicated below.

Proximate Analysis
The proximate analysis was conducted following the AOAC method [21], encompassing assessments of moisture content, ash content, fat content, and protein content.After obtaining the results for these four parameters, an examination of carbohydrate levels was performed using a distinct approach.

Texture Analysis
Texture analysis was conducted employing the Brookfield Engineering Labs, Inc. Texture Analyzer tool, utilizing the Texture Pro CT V1.2 type.Build 9.The chosen probe for the analysis was TA 39 with TA-BT-KI fixture and a 4500 g load cell.The instrument was configured with a target of 10 mm and a trigger load of 4.5 g.Test speed was set at 0.5 mm/s, while the return speed was set at 0.5 mm/s.Typically, one cycle was performed with a pre-test speed of 2 mm/s and a standard rate of 10 points/s.

Organoleptic Analysis
A total of twenty-five untrained panel members took part in organoleptic assessments, employing a five-point preference scale for the investigation.The parameters evaluated included colour, aroma, taste, texture, and overall acceptance, with scores ranging from 1 for "very dislike" to 5 for "extremely like."

Microstructure Analysis
Prior to testing, the samples underwent preparation and were coated with gold using an Ion Sputter tool (Hitachi E-1045) with parameters I=30 mA and t=10s.Subsequently, the SEM Jeol JSM-IT200 at 15 kV and Std.PC 40 was utilized to conduct the tests on the samples.

Specific Expansion Capability
The analysis of characteristics in gluten-free corn cookie products encompasses evaluations such as product development ratio, colour, proximate composition, organoleptic properties, and texture.The product development ratio indicates favorable expansion capacity and porosity, aligning with the expected acceptance levels for commonly consumed cookies.This ratio considers the development of thickness to weight and the development of diameter in comparison to weight.The outcomes of the gluten-free corn cookie development ratio are presented in Table 1 below.Significant variations were observed in the thickness-to-weight development ratio among different treatments, whereas the diameter-to-weight ratio did not exhibit statistically significant differences.
The gluten-free corn cookies with 1% HPMC addition recorded the highest value in terms of diameter development ratio, although statistically, the difference was not deemed significant.It's noteworthy that both baking conditions and the concentration of CMC played a significant role in influencing the quality attributes of cookies [25].

Colour Characteristic
The colour attributes of gluten-free corn cookies are determined by the values of L, a, b, and Hue.The analysis outcomes for these colour parameters are presented in the following Table 2.The colour parameter holds significant importance in assessing the overall acceptability of food products, including gluten-free cookies, by consumers [26].The colour characteristics of gluten-free corn cookies are determined by the values of L, a, b, and Hue.Across all parameters (L, a, b, and hue), the colour outcomes for gluten-free corn cookies exhibited statistically significant differences among various treatments.The dominant colour of the produced cookies is influenced by the yellow base colour of corn flour.The incorporation of food additives like CMC, MC, HPMC, and MCG contributes to alterations in the colour characteristics of the resulting gluten-free corn cookies.It's noteworthy that the overall cookie colour heavily relies on the colour of the primary flour used as an ingredient [27].In this instance, the use of yellow-coloured corn flour resulted in a relatively low WI value ranging from 62.13 to 69.00.The values of L, a, b, C, Hue, and WI collectively indicate substantial differences among the treatments.The physical appearance of cookies, influenced by the addition of various cellulose-derived food additives, is depicted in Figure 1 below.

Proximate Analysis
Based on the results of the analysis as shown in Table 3 below.To assess the chemical attributes of gluten-free corn cookies, a proximate content analysis was conducted, encompassing parameters such as moisture content, ash content, fat content, protein content, and carbohydrate content.The analysis outcomes indicated that the incorporation of cellulose-derived food additives led to distinct characteristics in terms of moisture content, ash content, fat content, protein content, carbohydrate content, and energy.The addition of CMC, MC, HPMC, and MCG at a 1% concentration resulted in statistically significant differences in the proximate parameter characteristics.
Typically, raw materials for corn flour exhibit a relatively high protein content of about 10.20% and a fat content of 1.55% [28].In a study by Herawati and Kamsiati [3], the proximate analysis of commercial corn flour revealed a protein content of 8.41% and a fat content of 0.89%.Cookies prepared by Helal and Afifi [29], with variations of corn flour and popcorn, showed protein levels ranging from 3.68% to 4.19%.The protein content in flour can vary due to factors such as plant variety, geographical cultivation area, growth period, and processing conditions [26].The formulation differences in the materials used can impact the resultant proximate content quality.

Texture Characteristic
Referring to the texture parameters, including hardness, adhesive force, adhesiveness, and springiness, the data is presented in Table 4 below.1872.67a0.17a 0.0000a 0.0000a Note: Numbers followed by different letters indicate significantly different with a 95% confidence interval To evaluate the texture quality based on the analysis results using a texture analyzer tool, the study employed texture analysis.The outcomes of the texture analysis for the parameters of adhesiveness, cohesiveness, and springiness did not reveal statistically significant differences.In contrast, the hardness parameter exhibited significant variations.The level of hardness is indicative of the crispness in the resulting cookies.Specifically, the addition of 1% CMC demonstrated the highest level of hardness compared to the control treatment and the addition of other types of cellulose derivatives.
According to Mir et al. [32], hydrocolloids can enhance the texture of gluten-free bread.The utilization of starch, gums, and hydrocolloids can lead to interactions influencing the texture of bakery products [33].Flour inherently contains fiber components that impact the texture of the final bakery products.The incorporation of hydrocolloid components, such as cellulose derivatives, is expected to contribute to the process of creating gluten-free cookies.
Incorporating starch, gum, and hydrocolloids into the formulation introduces interactions that can influence the texture of bakery products [33].Additionally, Luangsakul and Chiralaksanakul [34] emphasized that the type and concentration of sugar added can impact the texture of macarons.The formulation of materials plays a crucial role in determining the texture quality of the resulting dry bakery products.Another study highlighted that the hardness of cookies tends to increase with the inclusion of soluble fiber [35].
The texture of oven-dried biscuits primarily results from the starch gelatinization process, while in cold conditions, a arrangement forms due to the interaction between sugar and protein/starch [36].Seyhun et al. [37] mentioned that the level of firmness can rise with the recrystallization of amylose and amylopectin, the creation of complexes between starch and protein, and the redistribution of water among product components, along with other potential events that may occur post-baking or during storage.The combination of HPMC with banana flour enhances air micellar content and establishes a network resembling gluten.The hydrophobic groups in HPMC contribute to surface tension, thereby improving the cohesiveness of the dough system [38].

Organoleptic Test
The organoleptic evaluation conducted in this study encompasses sensory assessment parameters that represent the perceptions of the panelists.Sensory evaluation is a scientific and statistical approach designed to analyze human senses in order to assess product acceptability among consumers [30].The gluten-free corn cookies product underwent organoleptic analysis using a 5-point scale for preference levels, ranging from 1 (very dislikes) to 3 (neutral) and 5 (extremy like).The assessment covered parameters such as colour, flavor, taste, texture, and overall acceptance.The outcomes of the analysis are presented in The results of the organoleptic analysis for colour and texture parameters exhibited statistically significant differences.However, for the parameters of flavor, taste, and general acceptance, there were no statistically significant differences observed.The control group demonstrated a less favorable texture compared to the samples with the addition of cellulose-derived food additives.This suggests that the incorporation of cellulose derivatives enhances the texture, as perceived by the panelists in general.Even though the tool-based texture analysis revealed differences in hardness for cookies with 1% CMC, the organoleptic tests did not show significant distinctions across all parameters for cookies with cellulose derivatives.This implies that panelists provided holistic texture analysis responses rather than focusing on specific parameters like hardness alone.Fracturability, a crucial textural property, is highly important in the assessment of baked goods as it is closely linked to the human perception of freshness [31].This is particularly significant about the overall acceptability of cookies by consumers.To assess the porosity of gluten-free corn cookies, a microstructural profile analysis was conducted using a Scanning Electron Microscope (SEM).The microstructural porosity provides insights into the distribution of pores, both in terms of size and average distribution.The SEM analysis results indicate that the addition of food additives in the form of cellulose derivatives influences the porosity and distribution of the formed pores.As noted by Bourekoua et al. [39], the control samples exhibit a visible swollen starch structure on the rough surface compared to the compact structure in bread with the addition of hydrocolloids, which appears more amorphous and homogeneous.

Conclusion
Corn flour can be utilized in the preparation of gluten-corn cookies, with modifications achieved through the incorporation of cellulose-based food additives.The nature of cellulose derivative modification plays a crucial role in influencing attributes such as thickness/weight ratio, colour, proximate composition, organoleptic properties, and texture characteristics.Regarding adhesive texture parameters, there were no statistically significant differences observed in adhesiveness and springness.The highest level of hardness was observed in gluten-free corn cookies containing 1% CMC.Overall, the organoleptic test panelists expressed a favorable liking for all the gluten-free corn cookies.Subsequent research endeavors could focus on optimizing potential raw material sources for CMC production and exploring alternative opportunities for the utilization of local gluten-free food products.

Table 1 .
Ratio analysis results for the development of gluten-free corn cookies

Table 2 .
Results of colour analysis of gluten free corn cookies

Table 4 .
Gluten-free corn texture analysis results