Novel Mangosteen-Leaves-Based Marker Ink: Color Lightness, Viscosity, Optimized Composition, and Microstructural Analysis (2024)

2.1. Factors and Levels of the Design of Experiment

In the study, CMC and glycerol—designated as V₁ and V₂ respectively—were chosen as factors. Other factors, such as ferrous sulphate and benzalkonium chloride, were kept constant at 1 and 5 wt %, respectively. Five weight percent (5 wt %) denoted as 5% of the total weight of the leave’s boiled water. Factors and levels used in the DOE are shown in Table 1.

2.2. Design of Experiment

RSM was used to design and conduct experiments due to its lower experimental runs as compared to the conventional experiment. Table 2 shows the difference in the total number of experimental runs between full-design RSM and a full factorial design (classical method) based on five-level factors. The result shows that for analyzing four factors, the full-design RSM only requires a minimum of 30 experimental runs (with one replication) as compared to 625 for the full factorial design.

At each design stage, five levels and two factors were applied in the CCD and with three replications for a total of 39 experimental runs. The factors were selected based on preliminary lab work, their significant effect on the responses, and working range (workability). Table 3 displays the complete CCD with coded and uncoded levels of these factors. The value for the total block is 1 with the experiments carried out in randomized order. For analysis using RSM, V₁ = V₂ = 0 represent the center point. Replicating an entire DOE to increase the number of data points can be expensive and time-consuming. An alternative way to increase the accuracy of the analysis is to use center points. By increasing the number of center points in the DOE, the probability of analyzing data and perform prediction of the optimum value for the factors can be increased. Therefore, a total of 15 experimental runs has been designed for center points resulting in a total of 39 experimental runs.

The significance of the main factors and their interactions is calculated using the analysis of variance (ANOVA). The value of 95% was set as the significance level which reflected the p-value of 0.05. Based on the value of the correlation coefficient (R²), the regression coefficient model (mathematical model) developed in the ANOVA table is used for optimization purposes. Experimental data are fitted with a second-order polynomial model to obtain the regression coefficient model. The general mathematical model obtained from the analysis is shown in Equation (1)

where Y is the response, β₀, β_i, β_ii, and β_ij are regression coefficients for the intercept, linear, quadratic, and interaction terms, respectively. X_i and X_j are coded values for the independent variables [30].

The desirability function was used to optimize the central composite design. The desirability function was created in this study to minimize the viscosity and color lightness of the ink. Validation was carried out by triplicate under optimal conditions.

2.3. Raw Materials and Sample Preparation

Dry mangosteen leaves, used as the main component in the marker ink production, were obtained from the Family Fruits Farm, Batang Kali, Selangor, Malaysia. The CMC, ferrous sulphate, benzalkonium chloride, and glycerol used in this study was purchased from Merck KGaA, Darmstadt, Germany. The specification for glycerol is colorless, and it contains 1.0% water, viscous, and clear liquid. CMC is an odorless white powder with a viscosity of 400 to 800 centipoise (cp), in a 2% solution in water at 25 °C. Ferrous sulphate has a density of 1.898 g/mL at 25 °C while benzalkonium chloride is a clear, colorless liquid with a concentration of 50 to 55 w/w%. The marker ink was prepared by following the steps, as shown in Figure 1.

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Figure 1

Fabrication process of mangosteen-leaves-based marker ink.

Approximately 75 g of dry mangosteen leaves were first weighed by using a digital weighing scale (Mettler Toledo, Columbus, OH, USA) which was able to read up to 0.001 g and for a sample weight up to 220 g. These were then washed thoroughly and rinsed. Glycerol ranging from 15 g to 62.5 g was weighed by using a digital weighing scale and 375 mL of water was measured using a measuring cylinder, and both were mixed in a beaker and thoroughly stirred for 30 s. The mixture was boiled together on a hot plate (Thermo Fisher Scientific, Waltham, MA, USA) at a heating degree of 8 (circa. 300 °C) for 30 min to increase the extraction rate of dye from the leaves. The hot plate can be heated up to 350 °C and the heating rate can be set from 0% to 100% at 1% intervals. The beaker was covered with plastic foil, to reduce vapor evaporation. Once boiled, the heating degree was reduced to 2 (circa. 100 °C). After boiling the hot plate was switched off, and the boiled mixture was collected into a container using a strainer.

CMC, ferrous sulphate, and benzalkonium chloride of 1–12.5 g, 3 g, and 15 g, respectively were weighed using a digital scale and added into the boiled mixture containing mangosteen leaves. To avoid clumping, the mixture was thoroughly stirred with a whisker, resulting in a smooth and hom*ogeneous ink solution. The ink produced was stored in a glass container, sealed with an airtight cover, and kept in a cool, dry place for 24 h prior to testing.

2.4. Viscosity Test

The ink viscosity was investigated to develop a low viscous ink solution with a high drying rate. Ink samples were accordingly tested 24 h following preparation. The advanced AR-G2 rheometer (TA Instruments, New Castle, DE, USA) was used to conduct the viscosity test in accordance with the ASTM D-445 standard at 23 °C. A cone plate geometry with properties of 60 mm cone diameter, 1:0:0 cone angle ratio (deg:min:s), and 30 μm truncation was installed to the rheometer. The zero-gap was set for 30 µm and 5 g ink samples were placed on the Peltier plate by using a dropper. The experiment was initiated by clicking the ‘run’ icon, and the results were recorded.

2.5. Color Lightness Test

Color lightness was evaluated using a HunterLAB Ultrascan PRO d/8 Spectrophotometer (Hunter Associates Laboratory, Inc., Reston, VA, USA) operated in accordance with ASTM E1348. Approximately 50 mL of ink sample was used and placed in front of the porthole and the readings recorded. The colorimetric values were reported in terms of CIE color analysis for lightness (L*). The lightness, L*, represents the darkest black at L* = 0, and the brightest white at L* = 100.

2.6. Thermogravimetric Analysis

Thermogravimetric analysis (TGA) was conducted on marker ink samples using Mettler Toledo AG-TGA/SDTA (Model 851e, Mettler Toledo AG, Greifensee, Zürich, Switzerland). For specimen preparation, 20 mg of ink was used for each test. Nitrogen was used as a medium and the specimens were heated from 20 °C to 200 °C with a rate of 25 °C/min. Three ink samples that exhibited high, moderate, and low color lightness were tested to observe variation in their drying rates. As drying progressed, the weight of coating accordingly decreased due to solvent evaporation. The amount of solvent loss with time was monitored through mass change as recorded on the balance [31].

The drying rate of coating is the weight of solvent loss per time divided by the area of evaporation and this can be calculated using Equation (2) where R_mass is the evaporation rate, W is the weight of sample at a specific time, t is the time, ∆t is the time interval between measurements, and A is the evaporation area.

2.7. Microstructure of Rice Husk Ash

The scanning electron microscope (SEM) is one of the most versatile instruments available for the examination and analysis of microstructure morphology of plant materials [32]. Since the discovery that electrons can be deflected by a magnet, electron microscopy was developed by substituting the light source with a high-energy electron beam [33].

SEM analysis was carried out using the Hitachi S-3400N variable SEM. The microstructure images of mangosteen leaves, including raw samples, or those boiled without glycerol and with glycerol, and samples which exhibited high, moderate, and low color lightness and viscosity properties. Samples were prepared by placing on aluminum sample stubs with carbon conductive tape and were then sputter-coated with gold-palladium using Baltec SCD-005 Sputter Coater to produce high quality and bright image. The stub with coated samples was inserted into the sample chamber of the SEM for viewing.

Table 4

Design matrix and response value for the viscosity and color lightness test.

3.1. Statistical Analysis of Color Lightness and Viscosity Properties

A linear regression model was fitted to the experimental data using the least square technique. Several main parameters were considered in evaluating the statistical results, namely the coefficients of regression, the standard error of coefficient, and the p-value of each factor and its interactions for both responses which are color lightness and viscosity. The results in Table 5 indicated that all factors and interaction effects were highly significant (p < 0.000) except for V₂ with p < 0.113 and ‘V₂* V₂′ with p < 0.529. Values for R² = 0.9873 and R² (adjusted) = 0.9858 were considerably high, which indicated that 98.73% of sample variation in the response was attributed to the factors.

For viscosity, the p-value for both factors (color lightness and viscosity) and their interactions were considered significant at below the confidence level of 95% (p of 0.050). The results shown in Table 6 indicated that all factors and interaction effects were significant. The p values of all factors and their interactions were highly significant (p < 0.000) except for V₁ which did not affect the viscosity of the ink (p < 0.382). Values for R² = 0.9292 and R² (adjusted) = 0.9209 were considered very high, which indicated that 92.92% of the sample variation in the response was attributed to the independent variables.

Equations (3) and (4) represent the regression models for the color lightness and viscosity, respectively.

where Y_COL and Y_VIS represent the responses which are color lightness and viscosity, respectively whereas V₁ and V₂ are the decoded values of glycerol and CMC, respectively. The regression models can be used to calculate and analyze the effect of factors on the properties of plant-based marker ink.

3.2. Effect of Factors on Color Lightness and Viscosity

ANOVA and regression models were used to analyze the effect of various factors on the properties of the plant-based marker ink. Contour plots were used for better illustration. Figure 2 and Figure 3 illustrate the effect of glycerol (V₁) and CMC (V₂) on the responses, respectively. The findings show that higher V₁ resulted in higher color lightness, and lower V₂ resulted in lower viscosity. Based on Figure 2, the color lightness of mangosteen-leaves-based marker ink decreased when the ratio of glycerol concentration in the ink formulation is approaching 5. This indicates that a low concentration of glycerol reduces the value of color lightness in the ink.

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Figure 2

Contour plot for the effect of glycerol and CMC concentration on the color lightness of mangosteen-leaves-based marker ink.

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Figure 3

Contour plot for the effect of glycerol and CMC concentration on the viscosity of mangosteen-leaves-based marker ink.

An increase in the amount of glycerol in a liquid may increase the boiling temperature of the liquid [19]. Glycerol is alcohol with low vapor pressure. It changes its colligative properties when mixed with water, increasing the boiling point and lowering the melting point of the solution. According to Kowalska et al. [34], an increase in boiling temperature from 20 to 80 °C (glycerol content of 30% and below) may consequently decrease the total dye extraction yield. The study also discovered that increasing the glycerol concentration from 30% to 80%, while maintaining the same boiling temperature reduced the amount of extracted anthocyanins, which is in conformance with the results obtained in this study. Anthocyanin pigments are known as natural colorants due to their wide range of colors and high solubility in aqueous media [35].

The contour plot in Figure 3 shows the effect of glycerol and CMC concentration on the viscosity of plant-based marker ink. At a glycerol concentration of 5, the viscosity decreases as the CMC concentration decreases. Ghannam and Esmail [16] investigated the rheological properties of CMC solutions in a concentration ranging from 1% to 5%. When the concentration was lowest, they observed Newtonian behavior, while at higher concentrations, they observed non-Newtonian behavior such as pseudoplastic, thixotropic, and viscoelastic behavior.

Similar results were obtained by Edali et al. [36], who investigated the rheological behavior of CMC solutions also at higher concentrations. They found that the solution possessed both non-Newtonian and viscoelastic properties. Other studies also concluded that the apparent viscosity of CMC solution increased with rising concentrations. The results were obtained from the flow curves of the CMC solutions at different concentrations plotted over a log–log scale. This rise in apparent viscosity is due to the increase in the interactions between the CMC molecules [37].

3.3. Optimization of the Responses

The optimum formulation of marker ink can be achieved with the combination of glycerol ratio = 5 and CMC ratio = 3, as shown in Figure 4. The desirability of optimization was calculated as 0.98495, indicating that all parameters were within the target, which was to obtain desirable ink properties.

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Figure 4

Optimization plot for glycerol and CMC.

The value of composite desirability was calculated at 0.98495, which is high and which proved that the prediction is accurate. It also indicates that all parameters were within the target of obtaining the desirable ink properties. The optimization was completed within a set of parameters. For color properties, the target and upper values were set at 24.7 and 29.0, respectively. The target and upper boundary values for viscosity properties were set at 0.001 and 0.7278, respectively.

3.4. Experimental Validation

From Table 7, it is clear that the average error for color lightness and viscosity were well below 15% at only 0.50% and 9.09%, respectively. It was concluded that the regression model established using this method was able to optimize accurately the values for the responses.

3.5. Microstructure Analysis of Mangosteen Leaves

Five samples were selected to determine the microstructure of mangosteen leaves and the drying properties of the marker ink. The samples were dried mangosteen leaves, boiled leaves without glycerol, and with glycerol showing low (sample S26), moderate (sample S19), and high (sample S35) value of color lightness. The sample was analyzed using an SEM.

Figure 5 illustrates SEM micrographs of dry mangosteen leaves at 100× and 500× magnifications. The former magnification shows an image with a relatively corrugated surface, in the form of wrinkles, developed on the leaf samples. The degree of surface corrugation was attributed to the drying process of the leaves at ambient temperature. The cell structure shrank slightly as a result of water evaporating from the leaves. The latter magnification shows no pores on the smooth surface of the dry leaves. This confirms that the leaves dried due to the evaporation of water at ambient temperature and not because of the influence of elevated temperature. In this stage, the drying shrinkage was closely related to the total volume of evaporated water [38].

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Figure 5

SEM micrographs of dry mangosteen leaves at 100× (left) and 500× (right) magnification.

Glycerol was found to exert the most significant effect on color lightness as compared to that of other additives. SEM scanning was conducted to investigate the effect of different amounts of glycerol on the microstructure of mangosteen leaves. Its addition will subsequently affect the amount of dye extracted from the leaves.

Based on Figure 6, the SEM micrographs of all samples showed corrugated leaf surface attributed to cell shrinkage. Figure 6a shows shrunken cells but with most of the cell wall structures remaining intact adjoining each other. Under high-temperature conditions, the leaves developed a folded cuticle on the adaxial epidermis layer [39]. Further magnification at 500× revealed a more definite structure of the leaf samples as compared to those under 100× magnification. Based on Figure 6b, boiled mangosteen leaves without glycerol showed good bonding between cell wall structures and considerably smooth surfaces. The dye was extracted from the leaves by passing it through the small pores between the cells. These pores were observed at the intercellular space, between neighboring epidermal cells. The moderate and large size of irregular oblong pores and disrupted orientation of membranes were formed due to heat stress during the boiling process.

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Figure 6

SEM micrographs of (a,b) boiled dry mangosteen leaves without glycerol, (c,d) sample S35, (e,f) sample S19, and (g,h) sample S26 at 100× and 500× magnification.

A few recent studies described the effect of high temperature on the anatomical and ultrastructural changes which occurred in the leaf preparations including its organization, the protective outer layer of epidermis and cuticle as well as stomata [40]. The result is in agreement with that of Salem-Fnayou, Bouamama, Ghorbel and Mliki [39] which proved that a high-temperature condition can result in the folded cuticle and disrupted cell wall organization on the adaxial epidermis layer.

The microstructures of Figure 6a,c were found to be quite similar since the cell wall structures were still intact and adjoining each other. However, it can be seen that cell wall structures in sample S35 in Figure 6c,d had collapsed in certain areas and small pores had developed. The occurrence was due to the highest amount of glycerol used in boiling the sample. At high concentrations, glycerol is capable of altering plant cell structure. However, the collapse of cell wall structures is not as severe as samples S19 and S26. Glycerol is generally used as a solvent in water to extract natural pigments. The alcohol also acts as a pre-treatment agent and affects the final color produced through improving color performance [41].

Figure 6e of sample S19 covered with a thin needle-like and small-sized collapsed cell wall structures which mostly covered the leaf surface. Sample S26, as seen in Figure 6g, showed the highest amount of collapsed cell wall when the least amount of glycerol was used in boiling. The sample, therefore, showed the most significant effect of glycerol and in agreement with Figure 2. The thicker cell wall structures in sample S26 as compared to that of sample S19 can be visualized based on the brightness of the aggregated structures. The formation of the large and thick cell wall structures was probably due to the agglomeration of the high amount of the collapsed small-sized cell wall structures. Due to the large surface area and strong attractive interaction between particles, the aggregation process must have occurred as similarly recorded by other researchers [42]. Aggregation caused the fracture mechanism to change, with the fracture initiating and developing from the aggregation center [43].

The findings suggest that a decrease in the amount of glycerol in boiled water may alter the cell wall structure of the leaves and subsequently increase the dye extracted. The role of glycerol as dye extraction solvent has two main effects: first, the weakening of the membrane structures of the cells in which the anthocyanin are stored in cell vacuoles, and second, the transformation of the extracted anthocyanin into their flavylium form, which is the most stable form [44]. This condition has been extensively used in technological processes to extract dye from other natural sources such as fresh berries and grape pomace [45].

3.6. Drying Properties of Marker Ink

The thermogravimetric analysis (TGA) is a suitable alternative method in determining the drying rate of a solution as measured through sample weight loss during a drying process [31]. The drying rate is affected by the viscosity of a fluid and the rate of evaporation of a solvent [46]. In this study, four ink samples tested exhibited low, moderate, high, and optimum color lightness and viscosity properties. To better visualize the weight loss of the ink samples during the TGA test, a graph of weight loss (in%) as a function of time was plotted as shown in Figure 7.

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Figure 7

Weight loss as a function of time of sample S35, S19, and S26.

The weight loss for all samples for the first 120 s was very minimal, with a maximum of approximately 4% loss recorded for sample S35. As the test temperature was increased the rate of 25 °C for every 60 s, the initial drying rate was increased in the first 50 °C. External factors of a volatile matter, including higher air velocity, lower air humidity, and higher air temperature contribute to the increase in drying rate [47]. The drying curve represents the loss of volatiles first by evaporation from a saturated surface above the ink film followed in turn by a period of evaporation from a saturated surface of gradually decreasing area and finally when the volatile compounds evaporate from the interior of the ink’s solid [48]. Sample S35 recorded the highest percentage of weight loss at 64.1% followed by sample S19 (55.8%), and S26 (53.4%). It can be concluded that the sample S35 with the highest viscosity showed the fastest drying time.

Figure 8 shows the drying rate curves as a function of time in seconds. The drying rates for samples S19 and S26 were comparable at between 0.01% and 0.13% per second. Sample S35 shows the fastest drying rate of approximately 0.15% per second over 420 s. Due to the low viscosity of sample S35, the diffusion of solvent molecules (water) proceeds at a faster rate than a higher viscosity sample which thus has a slower ability to evaporate [49].

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Figure 8

Weight loss as a function of time of sample S35, S19, and S26.

The slower drying rate of highly viscous samples is due to diffusional mass transport limitations in the particle phase, arising from the viscous phase of the particles or due to a combination of oligomer degradation and mass transfer limitations [49]. If a viscous phase is formed, the mixing within the particle bulk will be kinetically limited, and an equilibrium process cannot represent the gas-particle partitioning. The drying rate is mainly governed by the reversible decomposition of oligomers back to monomers [50].

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