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Abstract The use of anthocyanin as a source of naturaldyes has been increased due to itslack of toxicity. In this study, natural dyes from the mulberry fruits extracted under different operating conditions such as extraction time (2060 min), temperature (4080 0C) and mass of the mulberry (1025 g) by conventional extraction technique. Response surface methodology (RSM) with the help of Design Expert Version 7.1.6 (STATEASE Inc., USA) for optimization of the extraction process and evaluation of interaction effects of different operating parameters. The optimum conditions for dye extraction were 40 min, 60oC and 17.5 g for extraction time, temperature, and mass of the fruits, respectively. The efficiency of extraction under these optimum conditions was found 1.147%. Keywords: Anthocyanin, naturaldyes, mulberry, Response surface methodology (RSM) I. INTRODUCTION Dyesensitized solar cells (DSSCs) which are also called Graetzel cells are a novel type of solar cells. Their advantages are mainly low cost production, low energy payback time, flexibility, performance also at diffuse light and multicolored options1–5. DSSCs become more and more interesting since a huge variety of dyes including also natural dyes can be used as light harvesting elements which provide the charge carriers. Unlike synthetic dyesensitizers, natural ones are easy to prepare, cheap, nontoxic, environmentally friendly and fully biodegradable. Among natural pigments, three main families of compounds have been exploited as sensitizer in DSSCs: chlorophylls 6, 7, anthocyanins6, 8and betalains6. In this article we focused our attention only on anthocyanins. Anthocyanins are a very large group of redblue plant pigments, which naturally occurs in all higher plants. They are responsible for the coloration of flowers, fruits, fruit juice, wines, leaves, stems, bulbs, roots, etc. The main sources of anthocyanins are some vegetables such as blackberries, grapes, blueberries, eggplant, mango … A response surface methodology (RSM) based on statistical design of experiments (DOEs) is becoming increasingly widespread in several sciences such as analytical chemistry, engineering and environmental. Recently RSM have been used jointly for both modeling and optimization of nature dye extraction method 9. In the present study, anthocyanins from the mulberry fruits extracts under different operating conditions such as extraction time (2060 min), temperature (40800C) and mass of the mulberry (1025g) by conventional extraction technique. The RSM with the help of Design Expert Version 7.1.6 (STATEASE Inc., USA) use for optimization of the extraction process and evaluation of interaction effects of different operating parameters. II. EXPERIMENTS Extract of dye Mulberry fruits were purchased from a local supermarket in Hanoi, Vietnam. The extracts of mulberry fruits obtained from fresh fruit. The fruits cleaned and dried. The first, 20g of fresh mulberry put into 60ml of ethanol (Merck) in glass100ml. Mixture heated to a temperature extraction for 30 minutes. And then, Solution is filter more time with ethanol. At last, solution dries until mass constants. All samples protected from direct light exposure. Design of experiment Anthocyanin extraction parameters obtained by Mulberry fruits were optimized following the CCD and RSM. A 5level3factor central composite design wasemployed to evaluate the extraction parameters in this study.Twenty experiments were performed in a random order. The choice of given variables and their range were selected based on several outside sources and on preliminary studies in our laboratory. The range and coded level of the anthocyanin extraction process variables studied are listed in Table 1. Total of 20 experiments were set up using the CCD matrix. The yield extraction of mulberry values (Y) was taken as the response of the design experiment. Design Expert software version 7.0.0 (STATEASE Inc., Minneapolis, USA) was used for regression analysis of the experimental data and to calculate the effect of each variable and mutual effect. The responses (Y) of the anthocyanin extraction process were used to develop a quadratic polynomial equation that correlates the values of yield extraction as a function of the independent variables and their interactions as shown in the following Eq. (1): H_dye=β_o+∑_(i=1)k▒〖β_i x_i+∑_(i=1)k▒〖β_ii x_i2+〗〗 ∑_(i=1)▒∑_(j=1+i)▒〖β_ij x_i x_j+ε〗(1) where Hdye is the anthocyanin extraction yield value in mulberry fruit, β0 is the offset term, βi is the linear effect, βii is the squared effect, βij is the interaction effect, xi is the ith independent variable and xj is the jth independent variable. The developed model was tested with the analysis of variance (ANOVA) with 5% level of significance. The statistical significance of the secondorder model equation was determined by Fvalue. Plotting of response surfaces and contour plots were used to identify the optimum conditions of the extraction parameters.
EXTRACTION OF ANTHOCYANNIN FROM MUMBERY FRUITS: PROCESS OPTIMIZATION USING RESPONSE SURFACE METHODOLOGY (RSM) Lưu Thi Lan Anh1, Nguyen Thị Tuyet Mai2*, Tran Thanh Thai3, Trinh Xuan Anh2, Phan Trung Nghia2, Ta Ngoc Dung2, Huynh Dang Chinh2 and Vo Thach Son1 School of Physics Engineering, Hanoi University of Science and Technology, No1, Dai Co Viet, Hai Ba Trung, Hanoi, Vietnam School of Chemical Engineering, Hanoi University of Science and Technology, No1, Dai Co Viet, Hai Ba Trung, Hanoi, Vietnam Quy Nhon University, 170, An Duong Vuong Street, Quynhon, Binhdinh Abstract The use of anthocyanin as a source of natural dyes has been increased due to its lack of toxicity In this study, natural dyes from the mulberry fruits extracted under different operating conditions such as extraction time (20 ÷60 min), temperature (40÷80 0C) and mass of the mulberry (10 ÷25 g) by conventional extraction technique Response surface methodology (RSM) with the help of Design Expert Version 7.1.6 (STAT-EASE Inc., USA) for optimization of the extraction process and evaluation of interaction effects of different operating parameters The optimum conditions for dye extraction were 40 min, 60oC and 17.5 g for extraction time, temperature, and mass of the fruits, respectively The efficiency of extraction under these optimum conditions was found 1.147% Keywords: Anthocyanin, natural dyes, mulberry, Response surface methodology (RSM) I INTRODUCTION Dye-sensitized solar cells (DSSCs) which are also called Graetzel cells are a novel type of solar cells Their advantages are mainly low cost production, low energy payback time, flexibility, performance also at diffuse light and multicolored options[1]–[5] DSSCs become more and more interesting since a huge variety of dyes including also natural dyes can be used as light harvesting elements which provide the charge carriers Unlike synthetic dye-sensitizers, natural ones are easy to prepare, cheap, non-toxic, environmentally friendly and fully biodegradable Among natural pigments, three main families of compounds have been exploited as sensitizer in DSSCs: chlorophylls [6], [7], anthocyanins [6], [8] and betalains [6] In this article we focused our attention only on anthocyanins Anthocyanins are a very large group of red-blue plant pigments, which naturally occurs in all higher plants They are responsible for the coloration of flowers, fruits, fruit juice, wines, leaves, stems, bulbs, roots, etc The main sources of anthocyanins are some vegetables such as blackberries, grapes, blueberries, eggplant, mango … A response surface methodology (RSM) based on statistical design of experiments (DOEs) is becoming increasingly widespread in several sciences such as analytical chemistry, engineering and environmental Recently RSM have been used jointly for both modeling and optimization of nature dye extraction method [9] In the present study, anthocyanins from the mulberry fruits extracts under different operating conditions such as extraction time (20÷60 min), temperature (40÷800C) and mass of the mulberry (10÷25g) by conventional extraction technique The RSM with the help of Design Expert Version 7.1.6 (STAT-EASE Inc., USA) use for optimization of the extraction process and evaluation of interaction effects of different operating parameters II EXPERIMENTS Extract of dye Mulberry fruits were purchased from a local supermarket in Hanoi, Vietnam The extracts of mulberry fruits obtained from fresh fruit The fruits cleaned and dried The first, 20g of fresh mulberry put into 60ml of ethanol (Merck) in glass100ml Mixture heated to a temperature extraction for 30 minutes And then, Solution is filter more time with ethanol At last, solution dries until mass constants All samples protected from direct light exposure Design of experiment Anthocyanin extraction parameters obtained by Mulberry fruits were optimized following the CCD and RSM A 5-level-3-factor central composite design was employed to evaluate the extraction parameters in this study Twenty experiments were performed in a random order The choice of given variables and their range were selected based on several outside sources and on preliminary studies in our laboratory The range and coded level of the anthocyanin extraction process variables studied are listed in Table Total of 20 experiments were set up using the CCD matrix The yield extraction of mulberry values (Y) was taken as the response of the design experiment Design Expert software version 7.0.0 (STAT-EASE Inc., Minneapolis, USA) was used for regression analysis of the experimental data and to calculate the effect of each variable and mutual effect The responses (Y) of the anthocyanin extraction process were used to develop a quadratic polynomial equation that correlates the values of yield extraction as a function of the independent variables and their interactions as shown in the following Eq (1): (1) where Hdye is the anthocyanin extraction yield value in mulberry fruit, β0 is the offset term, β i is the linear effect, βii is the squared effect, βij is the interaction effect, xi is the ith independent variable and xj is the jth independent variable The developed model was tested with the analysis of variance (ANOVA) with 5% level of significance The statistical significance of the second-order model equation was determined by F-value Plotting of response surfaces and contour plots were used to identify the optimum conditions of the extraction parameters Table Independent variables and levels used for response surface design Independent variables Temperature Weight Time Units C gram III RESULTS AND DISCUSSION The model expressed by Eq (2) represents the anthocyanin extraction yield value in mulberry fruit (Hdye) as a function of temperature (A), weight (B) and extraction time (C): Hdye = 1.10 + 0.22*A + 0.19*B + 0.17*C - 0.15* A2 - 0.17*B2 - 0.19*C2 Range of factors Min Max A 40 80 B 10 25 C 20 60 are not significant As shown in Table 3, the model is a good significant with F-value of 1.14, and a sufficient probability value (0.0006) The lack of fit value (F-value: 2.03) for regression of Eq (2) is not significant Non-significant lack of fit is good and displays that the model equation was sufficient for predicting the yield extraction of the samples The effects of the extraction parameters such as temperature, weight and extraction time were investigated on the yield values The P- values show the significance of coefficients and are also important for understanding the relationship between the parameters According to the analysis of variance (Table 2) A (temperature), B (weigh) and C (extraction time) are the most significant parameters (Prob > F less) Symbol (2) The statistical significance of Eq (2) was controlled by F-test and the analysis of variance (ANOVA) for response surface quadratic model is given in Table Values of probability (P) > F less than 0.05 indicate that model terms are significant Values greater than 0.1000 indicate the model terms Table Analysis of variance (ANOVA) for the fitted quadratic polynomial model for optimization of mulberry fruit extraction parameters P -Value Source Sum of Squares Df Mean Square F - Value Prob > F Model 0.88 0.098 10.14 0.0006 A-Temperature 0.052 0.052 5.39 0.0427 B-Weigh 0.021 0.021 2.14 0.173 C-Time 0.038 0.038 3.91 0.0761 AB 1.426E-003 1.426E-003 0.15 0.7087 AC 5.073E-003 5.073E-003 0.53 0.4850 BC 3.200E-005 3.200E-005 3.316E-003 0.9552 A2 0.015 0.015 1.50 0.2482 B2 5.982E-003 5.982E-003 0.62 0.4493 C2 7.164E-003 7.164E-003 0.74 0.4091 Residual 0.097 10 9.650E-003 Lack of Fit Pure error Cor Total 0.092 5.000E-003 0.98 19 The 3D response surfaces and 2D contour plots (Fig 1, and 3) generated by Design Expert 0.010 5.000E-003 2.03 0.4991 software version 7.0.0 are the graphical representations of the regression equation Yield (a) (b) Weight Yield Yield Weight Temp Temp Fig.1.3D response surfaces (a) and 2D contour plots (b) showing the effects of weight and temperature when extraction time was at 40min Yield Time Yield Yield Time Temp Temp Fig.2 3D response surfaces (a) and 2D contour plots (b) showing the effects of extraction time and temperature when weight was at 17.5g Yield Time Yield Yield Time Weight Weight Fig.3 3D response surfaces (a) and 2D contour plots (b) showing the effects of weight and extraction time when temperature was at 600C They can visualize the relationship between the response and each variable, and the interactions between two tested variables The 3D response surfaces and their respective 2D contours can also find the optimum ranges of the variables for the maximum of the response The maximum predicted response indicated by the surface confined in the smallest ellipse in the contour diagram On the basis of medium optimization, the quadratic model predicted that the maximum yield was 1.15%, when the temperature was 600C, weight was 17.5g and extraction time was 40min, respectively To verify the predicted results, validation experiments were performed in triplicate Under the optimized condition, the observed experimental extraction yield was 1.147%, suggesting that experimental and predicted values (1.15%) were in good agreement N a Ludin, a M Al-Alwani Mahmoud, A Bakar Mohamad, A A H Kadhum, K Sopian, and N S Abdul Karim, Renew Sustain Energy Rev., vol 31, 2014, pp 386-396 IV CONCLUSION M R Narayan, Renew Sustain Energy Rev., vol 16, no 1, 2011, pp 208-215 This study proved that statistical experimental designs offer an efficient extraction yield optimization of mulberry fruits A maximum extraction yield of 1.15% was achieved with the following optimized factors: the temperature 600C, weight 17.5g and extraction time 40min Under the optimized conditions, extraction yield of mulberry fruits was1.15% Validation experiments were also carried out to verify the accuracy of the model, and results showed that the predicted value agreed well with the experimental values REFERENCES C.-Y Chien and B.-D Hsu, Sol Energy, vol 98, 2013, pp 203-211 N Asim, K Sopian, S Ahmadi, K Saeedfar, M A Alghoul, O Saadatian, and S H Zaidi, Renew Sustain Energy Rev., vol 16, no 8, 2012, pp 58345847 J Gong, J Liang, and K Sumathy, Renew Sustain Energy Rev., vol 16, no 8, 2012, pp 5848-5860 M Shahid and F Mohammad, J Clean Prod., vol 53, 2013, pp 310-331 G Calogero, I Citro, G Di Marco, S Armeli Minicante, M Morabito, and G Genovese, Spectrochim Acta A Mol Biomol Spectrosc., vol 117, 2014, pp 702-6 G Calogero, J.-H Yum, A Sinopoli, G Di Marco, M Grätzel, and M K Nazeeruddin, Sol Energy, vol 86, no 5, 2012, pp 1563-1575 K Sinha, S Chowdhury, P Das Saha, and S Datta, Ind Crops Prod., vol 41, 2013, pp 165-171 QUÁ TRÌNH CHIẾT CHẤT ANTHOCYANIN TỪ QUẢ DÂU TẰM: TỐI ƯU HÓA QUÁ TRÌNH CHIẾT SỬ DỤNG PHƯƠNG PHÁP BỀ MẶT ĐÁP ỨNG (RSM) Lưu Thị Lan Anh1, Nguyễn Thị Tuyết Mai2*, Trần Thanh Thái3, Trịnh Xuân Anh2, Phan Trung Nghĩa2, Tạ Ngọc Dũng2, Huỳnh Đăng Chính2, and Võ Thạch Sơn1 Viện Vật lý Kỹ thuật, Trường Đại học Bách khoa Hà Nội, Số Đại Cồ Việt Hà Nội, Việt Nam Viện Kỹ thuật Hóa học, Trường Đại học Bách khoa Hà Nội Số Đại Cồ Việt Hà Nội, Việt Nam Đại học Quy Nhơn, 170 An Dương Vương, Quy Nhơn, Bình Định Tóm tắt Anthocyanin thường sử dụng nguồn chất màu tự nhiên ngày gia tăng chất không độc Trong nghiên cứu này, khảo sát chiết chất màu tự nhiên từ dâu tằm điều kiện khác thời gian chiết (20÷60 phút), nhiệt độ chiết (40÷80 0C) khối lượng dâu tằm sử dụng (10÷25 g) Phương pháp bề mặt đáp ứng (RSM) với trợ giúp phần mềm Design Expert Version 7.1.6 (STAT-EASE Inc., USA) để mô tối ưu hóa trình chiết theo thông số nghiên cứu Điều kiện chiết chất màu anthocyanin tối ưu theo mô là: Thời gian chiết t = 40 phút, nhiệt độ chiết T = 60 oC and khối lượng dâu tằm chiết m = 17.5 g Hiệu suất chiết tối ưu đạt H = 1.15% Giá trị phù hợp với giá trị thực nghiệm H = 1.147% Từ khóa: Anthocyanin, chất màu tự nhiên, dâu tằm, phương pháp bề mặt đáp ứng (RSM)