Optimization of the aqueous extract process from mangosteen peel for dyeing silk - Hong Phuong Pham Thi

Journal of Science and Technology 54 (4B) (2016) 94-101 OPTIMIZATION OF THE AQUEOUS EXTRACT PROCESS FROM MANGOSTEEN PEEL FOR DYEING SILK Hong Phuong Pham Thi1, *, Linh Hoang Thi2, Trung Kien Tran3, Tan Vu Duc4 1Industrial University of Ho Chi Minh City, 12 Nguyen Van Bao, Ward 4, Go Vap District, Ho Chi Minh City 2Hung Yen University of Technology and Education, Khoai Chau District, Hung Yen Province 3Hanoi University of Science and Technology, 1 Dai Co Viet, Hai Ba Trung District, Ha Noi 4Hanoi Industrial Textile Garmanet University, Le Chi Commune, Gia Lam District, Ha Noi *Email: pthphuong1978@gmail.com Received: 15 August 2016 2016; Accepted for publication: 10 November 2016 ASBTRACT This research studied the juice extraction process from mangosteen peel with water solvent and the paramesters influencing on extraction process such as extraction temperature, extraction time and extraction ratio, and evaluating the juice of extract by determining extraction efficiency, color saturation of fabric and color fastness of silk fabric. The research results showed that the juice extracted from mangosteen peel can be used to dye silk fabric with high color strength and fastness. And the results of research will bring the efficiency of environmental, economy and society; and will meet urgent demands today. Keywords: silk, natural color, mangosteen peel, extracting and testing a natural plant dye. 1. INTRODUCTION Garcinia mangostana Linn is one of the local fruits of Viet Nam and the South Eastern area. Magosteen Rind has been used as a natural dye in textile applications so the component of the aqueous extraction of mangosteen contains a variety of compounds chromophore such as gartanin, BR-xanthone A, 3-isomangostin, α-mangostin, garcinon Dand other compounds. Moreover, the advantage of mangosteen peel is part of waste materials and mangosteen peel occupy 68 ÷ 70 % per mangosteen fruit [1, 2]. 2. MATERIALS AND METHODOLOGY 2.1. Materials Optimization of the aqueous extract process from mangosteen peel for dyeing silk 95 Silk fabric used was purchased from Nha Xa village, Moc Nam, Duy Tien, Ha Nam province, Vietnam; Silk fabric had fiber density of 40 g/m2, brightness L* 88.65. Mangosteen peel was collected from Lai Thieu, Binh Duong from March to August every year. Mangosteen peel was ground into small particles from 0.5 to 1 mm, moisture content 8.5 %. The extracts of Mangosteen peel had been preserved in Kalisortbate 1 % at room temperature for 2 weeks. 2.2. Methodology Effect of the aqueous extract process from mangosteen peel on silk fabric: The aqueous of mangosteen peel was extracted by water extraction and distillation. Investigated extract temperature was from 50 to 70 oC in 1 hour with ratio of mangosteen pulp/water of 1/5; the extract time were observed from 120 to 180 min at 80oC extraction for ratio of mangosteen pulp/water is 1/5; and the ratio of mangosteen pulp/water was extracted from 1/4 to 1/6 in 1 hour 30 minutes at 80 °C [1, 2, 3]. Dyeing silk fabric with aqueous extract from mangosteen peel: aqueous extract of mangosteen was mixed with water at the ratio of volume; heated up with the speed of 2÷3 °C/minute to 70 °C. The color intensities of dyed silk fabrics were determined on Minolta CR 300 colorimeter, Japan 73180167. The color fastness of dyed silk fabrics were tested by the standard of washing (ISO 105-C01) for the highest fastness levels 5 and the lowest fastness levels 1 [4]; and the properties of aqueous extracts and dyed silk fabrics were evaluated by spectroscopic analysis methods such as FT-IT, LC-MS and scanning electron microscope SEM. Factorial experimental design of the extraction process from mangosteen rind: The model selected for this study is orthogonal center of complex pattern. Three variables were selected to study as extraction temperature (oC), extraction time (minutes), extraction ratio (mangosteen rind/water). Y1 is extraction efficiency and Y2 is color saturation of fabric, Xi and Xj represents the variables or parameters: bj, bji and bjj characterize the impact of variables Y1 and Y2, which showed by magnitude and sign of coefficients. Each value of objective function will be used to build a mathematical model in which a correlation between objective functions influencing factors was studied, given the form of polynomial equation [5]: 3. RESULTS AND DISCUSSION 3.1. Building experiment models and regression equation for extraction conditions Building experimental matrix: Between the variable coding (Xi) and the real variable value (Zi,) chosing to study at different levels are interrelated via the following formula: in which: : Research value at 0 (rootlevel) : The range of variables studied, Hong Phuong Pham Thi, et al 96 : The value study at high level (+1) : The value study at low (–1) With orthogonal plan, α value arm of the matrix is determined by the formula (4) with investigate levels of three selection variables (Table 1) and encoding matrix of three selection variables (Table 2) Table 1. Limit and levels of three selection variables. Investigate Variables (Real Variables) Encoding Variables Unit Investigate Levels -1 0 +1 Temperature (Z1) X1 oC 50 60 70 Time (Z2) X2 min 120 150 180 Ratio (Z3) X3 % the volume of water in the extraction mixture 75 80 85 Table 2. Encoding Matrix of three selection variables. Experiments Encoding Variables Objective Function X1 X2 X3 Extraction Efficiency (Y1) Color saturation of fabric (Y2) n= 2k =8 1 -1.0 -1.0 -1.0 8.42249 22.6309 2 1.0 -1.0 -1.0 13.8845 26.0337 3 -1.0 -1.0 -1.0 765957 20.1894 4 -1.0 -1.0 -1.0 11.9843 25.8653 5 -1.0 -1.0 -1.0 9.23277 24.7244 6 -1.0 -1.0 -1.0 13.8958 26.2337 7 -1.0 -1.0 -1.0 9.85443 24.0709 8 -1.0 -1.0 -1.0 11.2249 25.5362 n= 2k =6 9 -1.353 0 0 7.23277 20.2164 10 1.353 0 0 11.5572 25.7254 11 0 -1.353 0 10.5714 23.8362 12 0 1.353 0 11.1398 24.5147 13 0 0 -1.353 19.2817 27.9945 14 0 0 1.353 20.915 28.8362 n 0 =3 15 0 0 0 23.839 30.2588 16 0 0 0 23.7057 30.358 17 0 0 0 23.399 30.3856 Optimization of the aqueous extract process from mangosteen peel for dyeing silk 97 Table 3. Results of extraction efficiency and color saturation fabric by orthogonal matrix level 2. Exp. X1 X2 X3 Temp. (oC) Time (min) Ratio (%) Extraction Efficiency Y1 Color Saturation of Fabric Y2 1 -1 -1 -1 50 120 75 8.42249 24.6309 2 1 -1 -1 70 120 75 13.8845 24.9337 3 -1 1 -1 50 180 75 7.65957 25.6894 4 1 1 -1 70 180 75 11.9843 25.8653 5 -1 -1 1 50 120 85 9.23277 24.0244 6 1 -1 1 70 120 85 13.8958 24.6337 7 -1 1 1 50 180 85 9.85443 24.4709 8 1 1 1 70 180 85 11.2249 25.8362 9 -1.353 0 0 46.47 150 80 7.23277 24.8164 10 1.353 0 0 73.5 150 80 11.5572 25.8254 11 0 -1.353 0 60 117.06 80 10.5714 25.8362 12 0 1.353 0 60 182.94 80 11.1398 25.8147 13 0 0 -1.353 60 150 73.235 19.2817 26.9945 14 0 0 1.353 60 150 86.765 20.915 25.8362 15 0 0 0 60 150 80 23.839 27.2588 16 0 0 0 60 150 80 23.7057 27.358 17 0 0 0 60 150 80 23.399 27.3856 The maximum values of two objective functions be used to build mathematical models (1). Extraction efficiency and color saturation of fabric obtain from experiments (Table 3). From the results of color saturation of fabric and software Statgraphics Centurion XV.II, carried out statistical analysis correlation and regression to determine the regression of the process, checked conformity of the mathematical model to find the optimal conditions for extraction extracts from mangosteen peel. Then carried out analyze and appreciate the influence of the investigate variables to extraction efficiency of the extraction process and color saturation of fabric, and determine the optimal variables of the process. Analysis of variance and regression: The Pareto Fig. 1 showed that the effect of investigate variables to extraction efficiency of the extraction process and color saturation of fabric in which the letters A, B, C represent encoding variables: X1, X2, X3. The impact level of investigate factors of the extraction process was assessed by statistical analysis of experimental results. The column value showed the level of impact of factors quadratic and interaction of two variables simultaneously. The gray lines showed interaction effects on color saturation of fabric are positive effects (+) which increases extraction efficiency and color saturation of fabric. The blue lines are negative effects (-) which reduce extraction efficiency and color saturation of fabric. The value ratio of F is high and index P is low, the regression coefficients are more meaningful and more significant impact. Hong Phuong Pham Thi, et al 98 (a) (b) Figure 1. The influence of investigate factors to extraction efficiency (a) and color saturation of fabric (b). Thus, Fig. 1 showed that the effect of factors type 1 (A, B, C) and interactive effects level 2 AA, BB, CC are substantial and are retained so F is high and P-unreliability value is lower 0.05 (ie. Reliability ≥ 95 %). The residual effects which no meaning were removed because P is higher 0.05. Table 4. The estimated value of regression coefficients. Factors Regression coefficients The value of regression coefficients Extraction Efficiency (Y1) Color Saturation of Fabric (Y2) Const b0 -526.414 -232.439 A: temp. b1 8.7853 4.87044 B: time b2 1.91145 0.664662 C: ratio b3 3.3449 1.4236 AA b11 -0.0634884 -0.0308128 AB b12 -0.00184578 0.000928792 AC b13 -0.00876112 -0.0142486 BB b22 -0.00616786 -0.00269266 BC b23 0.00047768 0.000979536 CC b33 -0.0175431 -0.00375685 Data processing by Statgraphics software obtained the regression with real variables (Z) và encoding variables (x) in Table 4. The objective function of Extraction Efficiency: Y1= –526.414 + 8.7853Z1 + 1.91145Z2 + 3.3449Z3 – 0.0634884Z12 – 0.00184578Z1Z2 – 0.00876112Z1Z3 – 0.00269266 Z22 + 0.00047768 Z2Z3 – 0.0175431Z32 (5) Ŷ1= 22.4966 + 1.8583x1 – 0.3381x2 + 0.383x3 – 6.348x12 – 0.5537x1x2 – 0.4691x1x3 – 5.55x22 –0.503x32 (6) The objective function of Color Saturation of Fabric: Y2 = -232.439 + 4.87044 Z1 + 0.664662 Z2 + 1.4236Z3 – 0.0308128Z12 + 0.000928792Z1Z2 – 0.0142486 Z1Z3 – 0.00616786Z22 + 0.000979536 Z2Z3–0.00375685 Z32 Ŷ2=29.5801+1.6727x1-0.2609x2+0.598x3-3.081x12+0.2786x1x2-0.763x1x3-2.42x22+0.157x2x3- 0.1077x32 Check the suitability of model by the standard of Fisher (fth)và Student (tα) with reappear variance S2th: is calculated based on the central experiments no= 3 and significance level α = 0.05, reappear freedom degrees fth=3-1=2. The correlation coefficient value (R2=95.701) Optimization of the aqueous extract process from mangosteen peel for dyeing silk 99 indicating that 95.701 % variations of extraction efficiency are due to impact of independent variables and 4.299 % are due to external factors which unexplained by the model. Likewise, the correlation coefficient value (R2=92.3481) indicating that 92.3481 % variations of Color Saturation of Fabric are due to impact of independent variables and 7.6519 % are due to external factors which unexplained by the model. This showed that the significance of of the two objective functions is rather high. 3.2. Analyze level affecting of factors to extraction efficiency and color saturation of fabric Figure 2. The influence of the investigate factors to extraction efficiency (a) and color saturation of fabric (b). Effect of extraction temperature to extraction efficiency and color saturation of fabric: The extraction temperature factor contributeing to promote the process of dissolving of the substances in mangosteen peel and impact mainly to extraction efficiency and color saturation of fabric (Fig. 2). Color saturation of fabric increases with increasing temperature and reached the highest value at 60 °C. Temperatures bring positive effects to increase in temperature range 60- 70 oC. When temperature increase 70 oC then color saturation and intensity decrease reflected some regression level 2 (b11). Effect of extraction time to extraction efficiency and color saturation of fabric: Extraction time has a positive and significant impact to extraction efficiency and color saturation of fabric but lower. Time factor affecting level 2 to color saturation of fabric reflected regression coefficient b2 in equation (5 and 7). Color saturation of fabric is obtained maximum value at 150 minutes; the study showed it is about time enough to completely dissolve the substances in mangosteen peel in extraction process. As the temperature factor is higher when the time 150 minutes, the color intensity reduction reflected by the regression coefficient level 2 (b22). Effect of extraction ratio of extraction efficiency and color saturation of fabric: The results of analysis showed that the percentage discount services can also influence the intensity level 2 to color fabric, but the effect of extract ratio decreased color intensity fabric and bring negative effects resulting from the regression equation (5 and 7) to the value of coefficient b3. In this study, with extraction ratio 1/4-1/6, extraction efficiency and color saturation of fabric increased and obtained the maximum value in center survey then decrease; this is due to extraction ratio increasing, excess water will dilute some chromophore compounds in mangosteen peel powder. Result optimization: From the regression equation obtained, optimization conditions mangosteen extract by software Statgraphics. Conditions of optimal extraction have received: color saturation of fabric 30.08; extraction temperature at 61.4 oC; extraction time 149.2 minutes and Hong Phuong Pham Thi, et al 100 84.6342 % mixed water respectively with extraction ratio 1/5. Carried out dye silk fabric with the optimal extraction process, check the color fastness indicators are achieved level 4-5/5. 3.3. Reviewed optimization results ( a) b) c) d) Figure 3. The results of FT-IR infrared spectroscopy and chromatography coupled mass spectrometry MS of extracts before and after dyeing. (a) (b) Figure 4. SEM results of silk fabric before and after dyeing with extracts from mangosteen peels. The FT-IR spectral results in Figure 3 (a) and 3 (b) found that absorption spectrum appears chemotherapy ranged OH, C≡C; C=O, a perfect fit with linking group of mangosteen ingredients in prior studies [1,2,3]. On the other hand, after dyeing with extracts, there are several slight differences from previous dye extracts, but at the peak change specific to chromophore (2102 cm-1; 1284; 1085; 1044 cm-1) so these groups have mounted color on canvas. At the same time, the results capture MS spectrum of optimized extracts in Figure 3 (c) and 3 (d) have also noticed the appearance of a lot of components in the extract chromophore as α-mangostin; β-mangostin; γ-mangostin (M = 409.3 g/mol), Acid galic (M = 169.3 g/mol), Gartanin (M = 396.45 g/mol), 3- isomangostin (M = 409.3 g/mol), cyanidin (M = 288.4 g/mol), Xanthone (M = 196.9 g/mol). And after dyeing service spectrum we can see loss of some compounds as α-mangostin, β- mangostin, γ-mangostin, acid galic, 3-isomangostin, this can be confirmed that compounds of chromophore have linked on silk fabrics. On dyed silk fabricl: The SEM results in Figure 4(a) and 4(b) of silk fabrics before and after dyeing with extracts from mangosteen peel at the same resolution showed appearance of some part tiny particles bind and fill the small slot on fiber surface; while there is a thin film on fiber after dye surface, fabric before dye is none. This proves that the chromophore element linked on silk fabrics makes surface structure of silk fabrics changes. Optimization of the aqueous extract process from mangosteen peel for dyeing silk 101 4. CONCLUSION The results of optimum extraction conditions were obtained temperature at 61.4 oC, time 149.2 minutes and percent of extract ratio is 84.6342 % (1/5). 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