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Tạp chí khoa học Công nghệ và Thực phẩm: Tập 22 - Số 4/2022

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Tạp chí khoa học Công nghệ và Thực phẩm: Tập 22 - Số 4/2022 trình bày các nội dung chính sau: Nghiên cứu xây dựng quy trình nhân giống in vitro cây trầu bà cung đàn (Philodendron ‘Jungle boogie’); Ảnh hưởng của chất điều hoà sinh trưởng thực vật đến quá trình nhân giống in vitro cây ba kích (Morinda officinalis How.); Nghiên cứu điều kiện chiết coumarin từ lá đơn đỏ (Excoecaria cochinchinesis);... Mời các bạn cùng tham khảo để nắm nội dung chi tiết của tạp chí.

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  1. TẠP CHÍ KHOA HỌC CÔNG NGHỆ VÀ THỰC PHẨM Tập 22 - Số 4 (12/2022) MỤC LỤC 1. Tran Thi Kim Nhan, Nguyen Thi Hai Hoa, Hoang Thi Ngoc Nhon - 3 Optimization of enzyme-assisted extraction of flavonoid from Glinus oppositifolius. 2. Bui Thi Phuong Quynh, Le Thi Kim Anh, Tran Nguyen An Sa - 12 Comparison of catalytic activities of magnetic iron oxides in phenol degradation. 3. Truong Thi Dieu Hien - Potential of spent coffee ground in 20 Pleurotus sajor-caju cultivation. 4. Lê Thị Thúy, Huỳnh Tuấn Qui, Trần Uyển Nhi - Nghiên cứu xây 28 dựng quy trình nhân giống in vitro cây trầu bà cung đàn (Philodendron ‘Jungle boogie’) 5. Trịnh Thị Hương, Nguyễn Ngọc Hoàng Vân, Trần Trọng Tuấn - Ảnh 37 hưởng của chất điều hoà sinh trưởng thực vật đến quá trình nhân giống in vitro cây ba kích (Morinda officinalis How.). 6. Mai Minh Trẫm, Phạm Thị Cẩm Hoa, Hoàng Thị Ngọc Nhơn - 47 Nghiên cứu điều kiện chiết coumarin từ lá đơn đỏ (Excoecaria cochinchinesis). 7. Nguyễn Đào Thanh Hương, Hồ Thị Nguyệt, Trương Minh Ngọc - 55 Ảnh hưởng của một số điều kiện chiết xuất đến hàm lượng polyphenols và flavonoids thu được trong dịch chiết lá cây Costus pictus D. Don trồng tại Việt Nam. 8. La Bội Sương, Nguyễn Cẩm Hường, Hoàng Thị Ngọc Nhơn - Tối 64 ưu điều kiện trích ly lutein có hỗ trợ siêu âm từ lá đinh lăng Polyscias fruticosa (L.) Harms. 9. Đỗ Thị Mai Trinh, Trương Minh Ngọc, Nguyễn Thị Liên, Nguyễn 76 Thị Hạnh - Tối ưu hóa điều kiện tách chiết saponin triterpenoid từ bã hạt cây sở (Camellia oleifera) bằng phương pháp đáp ứng bề mặt (RSM). 1
  2. 10. Nguyễn Công Bỉnh, Đinh Hữu Đông, Trần Thị Phương Kiều, Đào 88 Thị Tuyết Mai, Trần Quốc Đảm - Tối ưu hóa điều kiện thủy phân collagen từ da cá ngừ vây vàng (Thunnus albacares) theo mô hình Box-Behnken. 11. Trần Thị Ngọc Mai, Trần Thị Thúy Nhàn, Trương Thị Diệu Hiền - 97 Nghiên cứu nâng cao hiệu quả xử lý antimony trong nước thải nhà máy sợi. 12 Phạm Duy Thanh, Nguyễn Mậu Trung Chính, Phạm Thị Ngọc Hân, 105 Phùng Lê Thúy Hằng, Nguyễn Lan Hương - Nghiên cứu khả năng xử lý nước thải chăn nuôi heo sau xử lý kỵ khí bằng quá trình tăng trưởng dính bám của Spirulina platensis có hỗ trợ chiếu sáng bằng đèn LED. 13. Lê Minh Thanh, Nguyễn Hữu Sự, Ngô Hoàng Ấn - Phân tích và đánh 115 giá hiệu năng của NOMA-CRN sử dụng học sâu. 14. Bùi Quốc Tú, Nguyễn Huy Hoàng, Trương Quang Phúc, Lê Quang 132 Bình, Hồ Nhựt Minh - Nhận diện biển báo và tín hiệu đèn giao thông sử dụng YOLOv4 trên phần cứng Jetson TX2. 15. Mai Văn Lưu, Nguyễn Thanh Vân, Nguyễn Thuỳ Trang - Ảnh hưởng 143 của độ rộng xung bơm lên biến đổi quang nhiệt trong hoạt chất laser rắn. 16. Nguyễn Quốc Tiến, Đào Thị Trang - Tổng quan về môđun nội xạ và 149 các mở rộng của nó. 17. Vũ Văn Quế - Sáng tạo, đổi mới, bản lĩnh của Hồ Chí Minh trong 156 tác phẩm “Sửa đổi lối làm việc”. 2
  3. Journal of Science Technology and Food 22 (4) (2022) 3-11 OPTIMIZATION OF ENZYME-ASSISTED EXTRACTION OF FLAVONOID FROM Glinus oppositifolius Tran Thi Kim Nhan, Nguyen Thi Hai Hoa, Hoang Thi Ngoc Nhon* Ho Chi Minh City University of Food Industry *Email: nhonhtn@fst.edu.vn Received: 17 May 2022; Accepted: 15 June 2022 ABSTRACT Glinus oppositifolius, a potential medicinal herb used in many countries around the world, contains lots of bioactive compounds. One of the essential ingredients was flavonoid, a group of natural compounds that have many beneficial effects on human health, such as antioxidant functions, antibacterial, anti-inflammatory, and anti-cancer. The independent variables, including enzyme concentration (10-50 UI/g), temperature (50-70 °C), and time (60- 120 min), were investigated. The flavonoid extraction conditions were optimized with the CCD (Central Composite Design) design by response surface method (RSM). The results indicated that the optimal extraction conditions were found to be enzyme concentration (24.12 UI/g), temperature (68 °C), and time (99.8 min). Under such conditions, the highest content of flavonoid is 26.13 ± 0.05 mg/g of dry matter. These results suggest that enzyme treatment could help extract valuable components such as flavonoids that hold good potential for use in the food, cosmetic and pharmaceutical industries. Keywords: Cellulase enzyme, extraction, flavonoids, Glinus oppositifolius. 1. INTRODUCTION Glinus oppositifolius, an herbaceous plant with slender stem and branches, grows widely in Vietnam and tropical areas of Asia, Africa, and Australia [1]. It is distributed along with the coastal provinces, from the Hong River to the Mekong Delta in Vietnam. It is used as a vegetable and a precious medicine to treat some diseases. The extract has beneficial effects on digestion, aperitif, antibiotic, liver laxative, mouth sores, periodontitis, bleeding teeth, and diuretic [2]. Its extract has long been used as an antipyretic agent in traditional medicine for liver disease and jaundice. The active ingredients in this herbal medicine have been extracted and used in combination with other medicinal herbs to make soft capsules or tablets for modern medicine. It is known that G. oppositifolius has a prosperous chemical composition (alkaloids, saponins, steroids, anthocyanins, etc.) and especially contains large amounts of flavonoids with many important biological activities. Flavonoid, a natural yellow pigment synthesized from phenylalanine [3], is a natural compound found in plants. More than 6000 flavonoids have been founded in vegetables, seeds, and fruits [4]. They reveal multiple positive effects because of their antioxidant and free radical scavenging action. So, it is beneficial for human health. This compound also has anti- inflammatory effects, antiviral or anti-allergic, and a protective role against cardiovascular disease, cancer, and various pathologies [5]. 3
  4. Tran Thi Kim Nhan, Nguyen Thi Hai Hoa, Hoang Thi Ngoc Nhon Figure 1. Glinus oppositifolius In recent years, enzyme techniques have been increasingly interesting in studies on extracting bioactive compounds from plants. Enzyme-assisted extraction offers a safe, green, and novel approach to extracting bioactive compounds. This technique is also safe for targeted substances and users in both laboratory and industrial conditions [6]. However, their recovery from the plant matrix is generally limited by the presence of a physical barrier (cell wall). Thus, the use of novel extraction procedures to enhance their release is essential. Thus, the enzyme-assisted extraction method seems suitable for obtaining and applying bioactive substances such as flavonoids from plants such as G. oppositifolius. Therefore, this work aims to assess the potential use of cellulase to improve the extraction efficiency of bioactive compounds from G. oppositifolius, and to find out and optimize the flavonoid extraction conditions from the material to offer a foundation for further studies on applying this compound in practice. 2. MATERIALS AND METHODS 2.1. Materials Fresh G. oppositifolius in green was collected in Chau Phu district, An Giang province, in July 2021. After being harvested, G. oppositifolius would be cleaned by washing to remove impurities. The leaves were dried at 60 ºC until under 10% moisture. The fine powder was obtained by grinding by a mechanical grinder (less than 80 mesh size) and stored in PE bags, protected from light and powder for the experiments. Chemicals such as sodium carbonate (Na2CO3), sodium nitrite (NaNO2), aluminum chloride (AlCl3), sodium hydroxide (NaOH), and methanol 99.5% were procured from Fisher Scientific (USA). Quercetin was purchased from Sigma-Aldrich Chemie GmbH (Steinheim, Germany), and cellulase (10000U/g) from Antozyme Biotech Pvt.Ltd (India). 2.2. Methods 2.2.1. Effects of enzyme-assisted extraction 1g of raw materials (calculated by dry matter-dm), adding water as a solvent with the ratio of material/solvent 1/30 (w/v). The extraction process was conducted with the support of cellulase at the pH range investigated (3, 4, 5, 6, 7), and the concentrations of the studied enzyme (10, 20, 30, 40, 50 UI/g) at the temperature (40, 50, 60, 70, 80 ºC) in the period of (30, 60, 90, 120, 150 minutes). Then, the mixture was centrifuged at 5500 rpm/5 min. After centrifugation, the solution was filtered through Whatman No.1 filter (China) to collect the filtrate. Then, the total flavonoid content (TFC) content was determined by UV-Vis 4
  5. Optimization of enzyme-assisted extraction of flavonoid from Glinus oppositifolius spectrophotometer (Genesys 10s thermo, Made in the USA) to select the appropriate conditions for the flavonoid extraction. 2.2.2. Experimental design RSM is a proper statistical and mathematical technique to evaluate multiple independent variables on the dependent variable and thus estimate the maximum yield of the process under a specific limited condition. The central composite design (CCD) is a common method to design experiments for building a quadratic model in RSM with response variables. CCD contains an embedded or fractional factorial design with a center point augmented with a group of new extreme values (low and high) for each factor in the design to allow curvature estimation, and the experimental matrix was built using JMP 10 software. Three independent variables include enzyme concentration (X1), temperature (X2), and time (X3). The marginal values and experimental design with independent variables, their ranges, and 20 experiments (6 experiments at the central point) were carried out randomly to optimize the extraction process. 2.2.3. Total flavonoids content determination Total flavonoid content was measured by the aluminum chloride colorimetric assay (Zhishen et al. 1999) using quercetin as a standard flavonoid. 1 mL of the extract was added to 4 mL of distilled water, and 0.3 mL of 5% NaNO2, and the mixture was incubated at room temperature for 5 min. After incubation, the mixture was treated with 0.3 mL 10% AlCl3 solution. After 1 min, 2 mL of 1 M NaOH was added, and 2.4 mL distilled water was added to the solution. The solution was mixed well, and the absorbance was measured at 415 nm against blank. The assay was performed based on the 6-point standard calibration curve of quercetin. The TFC was expressed as quercetin equivalents (QE) in milligrams per gram of dry material [7]. 2.2.4. Experimental design and statistical analysis The experiments were repeated three times. The results were presented as mean ± SD. Using IBM SPSS Statistics 20.0 software to analyze experimental data and evaluate the difference between samples (p< 0.05). JMP 10 software was used to analyze data in experimental optimization. The graph was drawn by Microsoft Excel 2016. 3. RESULTS AND DISCUSSION 3.1. Effects of enzyme and enzyme concentration on the flavonoids recovery yield The effects of cellulase on TFC are shown in Table 1. There is a significant difference between the samples treated with cellulase (19.93 mgQE/gdm) and the control (12.24 mgQE/gdm). Thus, the cellulase positively supported the extraction efficiency of flavonoids from G. oppositifolius. The extraction process was carried out with water as a solvent, ratio 1/30 (g/mL), pH 5 at 60 in 60 min. Table 1. Effects of cellulase on TFC Samples Flavonoid content (mgQE/gdm) Control 12.24 ± 0.65a Cellulase 19.93 ± 1.20b 5
  6. Tran Thi Kim Nhan, Nguyen Thi Hai Hoa, Hoang Thi Ngoc Nhon The enzyme concentration also significantly affected the obtained flavonoid content. According to Puri et al., the enzyme disrupted the cell wall and membrane to release bioactive components into the solvent with high-yield recovery during enzyme-assisted extraction [8]. Plant cell walls are complex and heterogeneous, mainly composed of cellulose, hemicellulose, and lignin. These components were considered barriers, hindering some compounds' extraction [9]. Enzymes cause break plant cells to be fully exposed to the solvent and hydrolyze polysaccharides and lipids, promoting the release of intracellular components [10]. From Figure 2, the obtained flavonoid concentration gradually increased with the increase of enzyme concentration and reached 23.70 mgQE/gdm at 20 UI/g. Then, the flavonoid concentration decreased from 30 UI/g to 50 UI/g (11.34 mgQE/gdm). The effectivity of enzyme-assisted extraction was affected by its concentration and substrate concentration. While low enzyme concentrations resulted in a slow reaction rate and incomplete process, the high enzyme concentration caused fast and thorough speed until a certain percentage of enzymes. Thus, too much enzyme was unchanged in extracted targeted components and wasteful of the extraction process. With the appropriate enzyme concentration, an enzyme- assisted extraction method was an excellent approach to enhancing extraction efficiency [11]. 30 Yields of flavonoids mgQE/gdm d 25 c c 20 b 15 a 10 5 0 10 20 30 40 50 Enzyme concentration(UI/g) Figure 2. Effects of enzyme concentration on TFC Note: Different letters a, b, c, and d in the same column represent statistically significant differences at p
  7. Optimization of enzyme-assisted extraction of flavonoid from Glinus oppositifolius amino acids [15]. On the other hand, the enzyme's active center would not be able to work well to break the cellulose chain in the plant cells at a low temperature. Therefore, the appropriate temperature for cellulase in this study was 60 °C. 30 c c Yields of flavonoids mgQE/gdm c 30 Yields of flavonoids mgQE/gdm c c b 25 25 b b 20 20 15 15 a a 10 10 5 5 0 0 30 60 90 120 150 40 50 60 70 80 Time (minutes) Temperature (oC) Figure 3. Effects of time extraction on TFC Figure 4. Effects of temperature extraction on TFC 3.3. Effects of different pH on extraction recovery yield of TFC The effects of pH on flavonoid extraction from G. oppositifolius are shown in Figure 5. The shape of an enzyme would be changed in a too acidic or too alkaline medium, which impacted the extraction efficiency [16]. The TFC content increased to 23.80 mgQE/gdm at pH 5. This figure continued to rise at pH 6, but there are no significant differences from that at pH 5. The results were consistent with the study of Pan et al. (2014) [17]. Therefore, pH 5 is considered a suitable condition for the following experiments. Each enzyme has its own optimal active pH range; changing the pH value from the optimal pH point reduces the enzyme's ability to work and even denatures it. This result is similar to the study of Yan et al. (2012) [18], investigating the effect of pH on the activity of cellulase enzyme-produced strains of the fungus Trichoderma reesei; pH 5 is the optimal pH for the best cellulose hydrolysis for this enzyme. 30 d d Yields of flavonoid 25 c mgQE/gCK 20 b 15 a 10 5 0 3 4 5 6 7 pH Figure 5. Effects of pH on recovery yield of TFC 3.4. The optimization of enzyme-assisted extraction of TFC According to the CCD complex model, the total flavonoid content obtained from different optimal conditions is presented in the modeling table. Based on suitable investigated conditions in the above single-factor experiments, the parameters such as enzyme concentration, temperature, and extraction time, were selected for the optimal study of extraction conditions to obtain the highest TFC content. The appropriate 7
  8. Tran Thi Kim Nhan, Nguyen Thi Hai Hoa, Hoang Thi Ngoc Nhon ranges of these factors are presented in Table 2. The optimal experiment was designed in CCD style by the RSM method. Table 2. Response surface central composite design and experimental flavonoids yield Independent variables No. Concentration Temperature Time Y (Yield of flavonoids, (UI/g) (C) (min) mgQE/gdm) 1 10 40 60 18.96 2 30 40 60 18.83 3 10 60 60 17.74 4 30 60 60 22.51 5 10 40 120 22.98 6 30 40 120 19.72 7 10 60 120 21.89 8 30 60 120 22.79 9 3.18 50 90 17.19 10 36.82 50 90 22.75 11 20 33.20 90 18.35 12 20 66.80 90 22.73 13 20 50 39.54 20.53 14 20 50 140.46 22.71 15 20 50 90 24.42 16 20 50 90 25.04 17 20 50 90 26.35 18 20 50 90 24.93 19 20 50 90 24.95 20 20 50 90 24.43 The factors with p < 0.05 were considered to influence the objective function, and the influencing factors with regression coefficients were determined by the multivariable regression method, obtained as follows: Y = 25.16 + 1.09X1 + 1.15X2 + 1.62X3 + 0.76X2X3 – 1.13X12 – 1.17X22 – 1.11X32 After conducting ANOVA analysis using JMP software, the following results were obtained: TFC obtained was 26.63 mgQE/gdm at optimal conditions with enzyme concentration (24.12 UI/g), temperature (68 °C), and time (99.8 minutes). The response surface model showed the influence of the investigated factors on the obtained total flavonoid content in the extract (Figure 6). The relationship between the repeat factors and flavonoids, while contour lines help visualize the shape of the response surface. Therefore, relying on surfaces helps assess the fit of the model [19]. 8
  9. Optimization of enzyme-assisted extraction of flavonoid from Glinus oppositifolius Figure 6. Response surface 3D (a, b, c) and 2D contour (d, e, f) plots showing the effect of different extraction parameters (X1: concentration, UI/g; X2: temperature, oC and X3 time, min) added on the response Y. Figure 7. The predictive model of TFC extraction For verification of the obtained parameters, experiments under optimized conditions were carried out (replicated three times). The obtained TFC of 26.13 mgQE/gdm, compared with the predicted TFC of 26.63 mgQE/gdm from the regression equation, accounting for 2.94% (
  10. Tran Thi Kim Nhan, Nguyen Thi Hai Hoa, Hoang Thi Ngoc Nhon UI/g), temperature (68 oC), and time (99.8 min). At optimal conditions, the TFC was maximized at 26.13 ± 0.05 mg/gdm. The results showed that G. oppositifolius extract contained a significant amount of flavonoids. The obtained results are mainly to find the optimal conditions for flavonoid extraction by cellulase enzyme to the maximum TFC content. More studies need to be conducted to obtain comprehensive characteristics of flavonoids from G. oppositifolius to apply to functional foods and pharmaceuticals. REFERENCES 1. Ridgway R. and Rowson J. - Glinus oppositifolius L. root - a substitute for senega, Journal of Pharmacy Pharmacology 8 (1) (1956) 915-926. 2. Mall T.P. and Tripathi S.C. - Exploitable vegetables for Food and health in Bahraich (UP) India, Agricultural Science Research Journal 6 (10) (2016) 241-246. 3. Harborne J.B. and Turner B.I. - Plant Chemosystematics, Academic Press, London, 1984. 4. Dixon R.A. and Pasinetti G.M. - Flavonoids and isoflavonoids: from plant biology to agriculture and neuroscience, Plant Physiology 154 (2) (2010) 453-457. 5. Chávez-González M.L., Sepúlveda L., Verma D.K., Luna-García H.A., Rodríguez- Durán L.V., Ilina A., and Aguilar C.N. - Conventional and emerging extraction processes of flavonoids, Processes 8 (4) (2020) 434. 6. Vergara-Barberán M., Lerma-García M., Herrero-Martínez J., and Simó-Alfonso E. - Use of an enzyme-assisted method to improve protein extraction from olive leaves, Food Chemistry 169 (2015) 28-33. 7. Simlai A., Chatterjee K., and Roy A. - A comparative study on antioxidant potentials of some leafy vegetables consumed widely in India, Journal of Food Biochemistry 38 (3) (2014) 365-373. 8. Puri M., Sharma D., and Barrow C.J. - Enzyme-assisted extraction of bioactives from plants, Trends in Biotechnology 30 (1) (2012) 37-44. 9. Khalil H., Lai T., Tye Y., Rizal S., Chong E., Yap S., Hamzah A., Fazita M., and Paridah M. - A review of extractions of seaweed hydrocolloids: Properties and applications, Express Polymer Letters 12 (4) (2018). 10. Nadar S.S., Rao P., and Rathod V.K. - Enzyme assisted extraction of biomolecules as an approach to novel extraction technology: A review, Food Research International 108 (2018) 309-330. 11. Panja P. - Green extraction methods of food polyphenols from vegetable materials, Current Opinion in Food Science 23 (2018) 173-182. 12. Duong Thi Ngoc Hanh and Nguyen Minh Thuy - The use of α-amylase enzyme in starch hydrolysis from Red rice, Scientific Journal of Can Tho University (2014) 61-67. 13. Hahn T., Lang S., Ulber R., and Muffler K. - Novel procedures for the extraction of fucoidan from brown algae, Process Biochemistry 47 (12) (2012) 1691-1698. 14. Phuong Nguyen Minh Nhat, Hoang Che Van, Binh Ly Nguyen, and Ai Chau Tran Diem - Effect of pectinase enzyme treament to juice yield and fermentation conditions to the quality of mango wine (Mangifera indica), Can Tho University Journal of Science 20 (2011) 127-136. 15. Al-Farsi M.A. and Lee C.Y. - Optimization of phenolics and dietary fibre extraction from date seeds, Food Chemistry 108 (3) (2008) 977-985. 10
  11. Optimization of enzyme-assisted extraction of flavonoid from Glinus oppositifolius 16. Nguyen Thi Ngoc Thuy, Nguyen Thi Thu Huyen, Truong Quang Duy, Phan Huynh Thuy Nga, and Tu Cao Thi Cam - Effect of solvent and pH value on extract of antioxidant activity compounds from perilla (Perilla frutescens) Journal of Science Techology and Food 14 (1) (2018) 66-74. 17. Pan S. and Wu S. - Cellulase-assisted extraction and antioxidant activity of the polysaccharides from garlic, Carbohydrate polymers 111 (2014) 606-609. 18. Zhong-Li Y., Xiao-Hong C., Qing-Dai L., Zhi-Yan Y., Yu-Ou T., and Juan Z. - A shortcut to the optimization of cellulase production using the mutant Trichoderma reesei YC-108, Indian Journal of Microbiology 52 (4) (2012) 670-675. 19. Baş D. and Boyacı I.H. - Modeling and optimization I: Usability of response surface methodology, Journal of Food Engineering 78 (3) (2007) 836-845. TÓM TẮT NGHIÊN CỨU TỐI ƯU HÓA CÁC ĐIỀU KIỆN TRÍCH LY FLAVONOIDS TỪ Glinus oppositifolius VỚI SỰ HỖ TRỢ CỦA ENZYME Trần Thị Kim Nhân, Nguyễn Thị Hải Hòa, Hoàng Thị Ngọc Nhơn* Trường Đại học Công nghiệp Thực phẩm TP.HCM *Email: nhonhtn@fst.edu.vn Rau đắng đất (Glinus oppositifolius) là một loại cây dược liệu tiềm năng được sử dụng phổ biến ở nhiều nước trên thế giới. Thành phần trong rau đắng đất chứa nhiều hợp chất hữu cơ mang hoạt tính sinh học, trong đó có flavonoid - nhóm hợp chất tự nhiên có nhiều tác dụng tốt cho sức khỏe con người, trong đó nổi bật nhất là các chức năng chống oxy hóa, kháng khuẩn, chống viêm nhiễm và ức chế tăng sinh của các tế bào ung thư. Để thu hồi được một lượng các hợp chất flavonoid ở mức cao nhất từ cây rau đắng đất flavonoids, nghiên cứu đã tiến hành trích ly kết hợp với sự hỗ trợ của enzyme cellulase trong quá trình trích ly flavonoids từ rau đắng đất và tối ưu hóa. Các thông số được khảo sát bao gồm: nồng độ enzyme (10-50 UI/g), nhiệt độ (50-70 oC), thời gian (60-120 phút). Điều kiện tối ưu trích ly flavonoids được thiết kế kiểu CCD (Central Composite Design) bằng phương pháp bề mặt đáp ứng (RSM), sử dụng phần mềm JMP 10. Kết quả nghiên cứu đã xác định được nồng độ enzyme, cùng nhiệt độ và thời gian trích ly tương ứng là: 24,12 UI/g, (68 °C) và 99,8 phút. Trong điều kiện tối ưu như thế có thể thu được 26,13 ± 0,05 mg/gck là điều kiện tối ưu để trích ly được hàm flavonoid cao nhất. Từ khóa: Enzyme cellulase, flavonoid, Glinus oppositifolius, rau đắng đất, trích ly. 11
  12. Journal of Science Technology and Food 22 (4) (2022) 12-19 COMPARISON OF CATALYTIC ACTIVITIES OF MAGNETIC IRON OXIDES IN PHENOL DEGRADATION Bui Thi Phuong Quynh, Le Thi Kim Anh, Tran Nguyen An Sa* Ho Chi Minh City University of Food Industry *Email: satna@hufi.edu.vn Received: 6 June 2022; Accepted: 5 September 2022 ABSTRACT Magnetic iron oxide-based materials have attracted great attention in catalysis due to their high activity, large availability, and easy catalyst collection and recycling. This work reports catalytic activities of magnetic iron oxides, which were synthesized via two different routes involving organic stabilizers, for the heterogeneous Fenton-like oxidation of phenol. Two kinds of catalysts, including crystalline Fe3O4 and amorphous nano-sized iron oxide particles, were formed according to the XRD and SEM data. Effects of reaction time, hydrogen peroxide amount, and solid catalyst on phenol degradation efficiency using the as-synthesized materials were investigated. The results showed that the synthesized crystalline Fe3O4 particles (1–5 μm) provided a higher overall phenol removal efficiency than the amorphous nano-sized iron oxide under similar reaction conditions. However, the initial oxidation rate was much faster by using the amorphous one. More than 98% phenol removal was obtained with the crystalline Fe3O4 after 60 min, while a similar efficiency was also achieved with the amorphous nano-sized iron oxide after 15 min but at significantly higher catalyst and H2O2 amounts. Keywords: Fenton reaction, phenol degradation, iron oxides, magnetic. 1. INTRODUCTION The great development of science and technology has a positive impact on the enhancement of human life quality these days; however, the world is also facing unexpected side effects of severe environmental pollution. Therefore, environmental protection and treatment have become a very urgent and important task for scientists and researchers worldwide. Phenols and phenol derivatives are very common pollutants discharged from various industrial processes such as petroleum refining, petrochemicals, production of pharmaceuticals, paper, plastics, coloring preparations, detergents, pesticides, and herbicides [1, 2]. To remove phenol compounds from wastewaters, a number of methods, including oxidation by oxygen in aqueous solution, electrochemical oxidation, adsorption, biodegradation, and Fenton (or Fenton- like) oxidation, have been studied and implemented [1, 3]. Recently, a heterogeneous Fenton-like process has emerged as a powerful solution for removing organic pollutants such as phenol and phenol derivatives. This process employed hydrogen peroxide and solid redox catalysts to degrade organic matters [4]. The catalytic decomposition of H2O2 results in the formation of hydroxyl (·OH) and per hydroxyl radicals (·HO2), which are robust oxidants to mineralize organic matters into H2O and CO2 [3]. Iron oxide-based Fenton catalysts have always received great interest for both research and practical applications, especially in environmental treatment, owing to their effectiveness, large availability, and reasonable cost [5]. Moreover, the magnetic ferric oxides are more advantageous for accessible collection and recycling of the used materials. Zelmanov et al. 12
  13. Comparison of catalytic activities of magnetic iron oxides in phenol degradation reported the high performance of iron oxide-based nanoparticles as catalysts for the degradation of ethylene glycol and phenol [6]. W. Wang et al. reported the synthesis and utilization of nano Fe3O4 materials, without using any surfactant or capping agent during the synthesis process, as a heterogeneous Fenton catalyst to remove phenol at a wide pH range [5]. In another work, Guohui Qi et al. studied phenol degradation in microbial fuel cells with a Fe3O4-reduced graphene oxide cathodic catalyst [7]. Many forms of iron oxides (such as goethite, hematite, magnetite, and ferrihydrite) have been found to be capable of transforming H2O2 into reactive free radicals. According to literature, this capacity is governed by some important properties such as surface area, particle size, and crystallinity. These properties depend essentially on the synthesis approach [8]. In this study, two synthesis routes were adopted to fabricate magnetic iron oxide catalysts and their application in the Fenton-like oxidation of phenol. Oxalic acid and polyvinyl pyrrolidone (PVP) were employed as stabilizers in the synthesis process as these substances contain groups that have a strong coordination affinity to ferric ions and thus possibly prevent them from aggregating into large crystals [9, 10]. The resulting materials were characterized using XRD and SEM. In application for phenol degradation, effects of reaction conditions including reaction time, hydrogen peroxide concentration, and catalyst amount, are investigated in detail. 2. MATERIALS AND METHODS 2.1. Chemicals Phenol (99%), oxalic acid (99,5%), hydrogen peroxide (30%), iron (II) sunfat heptahydrate. (99%), potassium ferricyanide (99,5%), 4-aminoantipyrine (99%), ammonia solution (25%), ammonium chloride (99,5%) and polyvinyl pyrrolidone (PVP) were purchased from Xilong Chemical Co.Ltd. (Shantou, China). 2.2. Synthesis of iron oxides In the first method, iron oxide was fabricated by using NH4OH as a precipitating agent and oxalic acid as an electrostatic stabilizer [9]. Firstly, a solution of 50 mL of H2O containing 2.28 g C2H2O4.2H20 was stirred, heated to 50 oC, and subsequently mixed with a solution of 50 mL H2O containing 5.56 g FeSO4.7H2O. Next, the ammonia solution was added drop-wise to the mixture. The received precipitates were washed several times with DI water until the pH reached the neutral value before being dried in an oven at 110 °C for 3 h. Finally, the powder was calcined at 300 °C for 2h and the resulting iron oxide was labeled S1. In another method, iron oxide was synthesized following the procedure previously used to fabricate Fe3O4 nanoparticles by J. Liu et al. [10]. A solution of 0.02 M NaOH, 2.78 g FeSO4.7H2O, and 1.5 g PVP was stirred and heated at 70 oC until the mixture was completely dissolved. Then, the solution was transferred to a thermostatic bath and stabilized at 70 oC for 2 h. The resulting suspension was centrifuged and collected precipitates were washed with ethanol and distilled water several times until pH reached the neutral value. Finally, the received powder was dried in the oven at 50 oC and the resulting iron oxide was labeled S2. 2.3. Evaluation of influencing factors Experiments for phenol degradation were performed as follows. A determined mass of iron oxides and a determined volume of H2O2 solution were added together to a 40 mL aqueous solution of phenol in a conical flask. The mixture was shaken for a predetermined time (KS260, German) and then the catalyst was separated from the solution by centrifugation at 5000 rpm for 5 min (HERMLE Z206A, German). The supernatant was collected for phenol analysis 13
  14. Bui Thi Phuong Quynh, Le Thi Kim Anh, Tran Nguyen An Sa referred to the Vietnam Standard TCVN 6216:1996 (ISO 6439: 1990). The procedure for analyzing phenol content in the sample is described as follows. A determined amount of phenol solution, which depended on the dilution factor, was mixed with 0.25 mL of pH = 10 buffer, 0.1 mL of 4-amino antipyrine solution and 0.1 mL of potassium ferricyanide solution to form red-orange complex. The solution was diluted in a 25-mL volumetric flask, left in dark for 10 min and then subjected to analysis (UV-Vis JENWAY 6305, wavelength of 510 nm). The calibration curve was constructed in the range 0.5-7 ppm. To examine the effect of time on catalyst performance, phenol treatment efficiency was measured at different times within 2h. The H2O2 volume was fixed at 35 µL. The catalyst mass was fixed at 0.05 g. Influence of H2O2 amount on treatment efficiency was examined in the H2O2 volume range 0–70 µL at the catalyst mass of 0.05 g and reaction time of 30 min. The influence of varying catalyst mass was examined at three points of 0.0250, 0.0500, and 0.075 g. The initial concentration of phenol solutions used for all experiments was fixed at 200 ppm (V = 40 mL). Each experiment was performed 3 times to get mean values. 2.4. Characterization of materials The scanning electron microscopy imaging was performed on a JSM IT-200 (Japan). X-ray diffraction analyses were performed with a D2 Phaser. Typical radiation conditions were 30 kV, 10 mA, Cu Kα radiation (λ = 1,54Ao) and 2 theta in range of 5 – 80o. These characterizations were conducted at Viet Duc Center- Ho Chi Minh City University of Food Industry. 3. RESULTS AND DISCUSSION 3.1. Characteristics of synthesized iron oxides The iron oxide received from the fabrication route S1 has a dark-brown color and was strongly attracted by a magnet showing a good magnetic property (Figure 1). The fabrication route S2 provided the yellow-brown oxide powder, which is likely in hydrated form. S2 was not as active as S1 under the effect of a magnet. The SEM image of S1 shows the presence of discrete Fe3O4 particles of 1–5 μm, while S2 has much smaller grains at nano sizes and some zones indicate the formation of large aggregates (Figure 2). Figure 1. Iron oxides received from the fabrication route 1 and 2 Figure 2. SEM images of S1 and S2 14
  15. Comparison of catalytic activities of magnetic iron oxides in phenol degradation The XRD pattern of S1 (Figure 3a) shows typical diffraction peaks of magnetite (Fe3O4) at 30.15o; 36.27o; 43.32o; 53.89o; 57.13o and 62.29o corresponding to the (220), (311), (400), (422), (511) and (440) crystalline planes, respectively [11]. In addition, small shoulders around 32o and 49o were detected and could be assigned to the presence of hematite α-Fe2O3 (JCPDS card No. 33-0664, 19-0629, and 70-1522 for hematite and magnetite, respectively). The XRD results indicate that the majority phase of S1 is magnetite with a small presence of hematite. This further explains why the powder does not have the typical black color of the pure magnetite but has a dark-brown color. A small number of iron species was possibly transformed to separate hematite phases during the calcination process. The dark-brown color of the mixture of hematite (minor phase) and magnetite (major phase) was also previously reported by N. Mufti et al. [12]. On the other hand, the amorphous phase is the major phase of S2 and the only crystalline plane of iron oxides was detected at around 35.8o (Figure 3b). Figure 3. XRD patterns of S1 (a) and S2 (b) 3.2. Catalytic performance in phenol degradation 3.2.1. Effect of reaction time For the Fenton-like reaction with S1 catalyst, the phenol degradation rate was fast in the first 15 min (from around zero level to 87%) and slowed down until remaining almost unchanged after 60 min (98.2%). Further increasing reaction time to 90 min did not considerably change the treatment efficiency (Figure 4). The degradation reaction with S2 occurred much stronger in the first 5 min and the efficiency fluctuated at about 69% from 15 min. S1 and S2 catalysts required 60 and 15 min to reach the highest degradation efficiency. Interestingly, although S2 had a more kinetic advantage at the beginning, S1 appeared more efficient in general as the final treatment efficiency reached about 93%, which is about 1.3 times higher than that obtained with S2. It can be explained that the smaller-sized grains of S2 (according to SEM image) contribute to the initial fast reaction rate but the majority of the crystalline phase (according to XRD pattern) allow for the higher overall catalytic performance of S1. This finding agrees well with the literature indicating the prevailing effect of crystallinity of iron oxide over the surface area on catalytic activity [8]. 15
  16. Bui Thi Phuong Quynh, Le Thi Kim Anh, Tran Nguyen An Sa S1 S2 100 80 Efficiency (%) 60 40 20 0 0 20 40 60 80 100 Time (min) Figure 4. Effect of time on phenol degradation efficiency 3.2.2. Effect of H2O2 amount The effect of increasing H2O2 volume from zero to 70 μL on phenol treatment efficiency is presented in Figure 5. In general, higher H2O2 content supports higher treatment efficiency for both catalysts. According to literature, higher content of H2O2 could promote more interaction between H2O2 and iron oxides, thereby generating more hydroxyl radicals active for phenol degradation via the following reactions [4]: Fe(II)surface + H2O2 → Fe(III) surface + •OH + HO (1) Fe(III)surface + H2O2 → Fe(III) surface(H2O2) (2) Fe(III) surface (H2O2)→Fe(II) surface + HO2• + H+ (3) According to the obtained results, 35 μL H2O2 is at least required for the two catalysts to achieve significant phenol degradation under the tested reaction conditions. For S1, the efficiency increased significantly when increasing H2O2 volume to 35 μL and a further addition to 70 μL did not change the efficiency. For S2, the efficiency increased gradually until 70 μL but a much stronger effect of H2O2 amount was observed in the range 0‒35 μL. Compared to the activity of S2, that of S1 was influenced more significantly in the H2O2 range 10–35 μL and reached a maximum level sooner. However, it should be noted that the excess H2O2 may also react with the hydroxyl radicals, thereby reducing the oxidizing capacity, when the H2O2 content is too high [13]. S1 S2 100 80 Efficiency (%) 60 40 20 0 40 60 0 80 20 H2O2 volume (L) Figure 5. Effect of H2O2 amount on phenol degradation efficiency 3.2.3. Effect of catalyst amount Effect of catalyst amount on phenol degradation efficiency was investigated at 0.025, 0.05 and 0.075 g (equivalent to 0.0625, 0.125 and 0.1875% (w/v)) with the results shown in Figure 6. 16
  17. Comparison of catalytic activities of magnetic iron oxides in phenol degradation The degradation efficiency improved significantly as the mass of the two catalysts increased from 0.025 to 0.05 g as a result of the presence of more active sites for the degradation reaction. Increases in the efficiency by nearly 23% and 30% were recorded for S1 and S2, respectively, when the catalyst amount doubled from 0.025 to 0.05 g. Further increase of the catalyst amount to 0.075 g, however, offered just a slight enhancement in the performance. These results show that the catalyst mass of 0.05 g, or the solid to solution ratio of 0.125%, is sufficient for phenol degradation under tested reaction conditions. S1 S2 100 80 Efficiency (%) 60 40 20 0 0,025 0,05 0,075 Catalyst mass (g) Figure 6. Effect of catalyst mass on phenol degradation efficiency 3.2.4. Reaction conditions for high removal efficiencies The reaction conditions for phenol degradation using the two catalysts, including the catalyst mass/solution volume ratio, H2O2/solution volume ratio, and required time to obtain more than 98% degradation efficiency (at phenol concentration of 200 ppm) are listed in Table 1. It can be seen that, in order to achieve nearly complete degradation of phenol, the crystalline Fe3O4 particles (S1) required much less H2O2 amount but a longer reaction time as compared to the amorphous nano-sized iron oxide (S2). Meanwhile, S2 is more advantageous in terms of shorter reaction time at the compensation of higher amounts of the catalyst or H2O2. Table 1. Comparison of the reaction conditions for two catalysts to achieve high phenol degradation activity Catalyst amount / Reaction time H2O2 ratio Removal Material solution volume (minimum required) (%, v/v) percentage (%) ratio (%, w/v) (min) Crystalline Fe3O4 0.125 0.0875 60 min 98.29 particles (S1) Crystalline Fe3O4 0.125 1.75 60 min 99.32 particles (S1) Amorphous nano-sized 0.125 2.625 15 min 98.41 iron oxide (S2) Amorphous nano-sized 0.1875 2.625 15 min 99.05 iron oxide (S2) 17
  18. Bui Thi Phuong Quynh, Le Thi Kim Anh, Tran Nguyen An Sa 4. CONCLUSION This study reports the synthesis of iron oxide catalysts for efficient phenol degradation by using two different synthesis routes. Two kinds of materials, including the crystalline Fe3O4 particles and the amorphous nano-sized iron oxide, were produced according to SEM and XRD data. Both catalysts were found to exhibit remarkable performance in the Fenton-like oxidation of phenol. The crystalline Fe3O4 particles required much less H2O2 but longer reaction time compared to the amorphous nano-sized iron oxide to achieve nearly complete degradation of phenol. On the other hand, the amorphous nano-sized iron oxide was more advantageous in terms of shorter reaction time. For approximate 99% removal of phenol, reaction conditions with the crystalline Fe3O4 were found at the catalyst /solution ratio of 0.125% (w/v), H2O2/solution volume ratio of 1.75%, and reaction time of 60 min. A similar efficiency was obtained with the amorphous nano-sized iron oxide at the catalyst/solution ratio of 0.1875% (w/v), H2O2/solution volume ratio of 2.625%, and reaction time of 15 min. REFERENCES 1. Said K.A.M, Ismail A.F., Karim Z.A., Abdullah M.S., Hafeez A. - A review of technologies for the phenolic compounds recovery and phenol removal from wastewater, Process Safety and Environmental Protection 151 (2021) 257–289. 2. Erylmaz C., Genç A. - Review of treatment technologies for the removal of phenol from wastewaters, Journal of Water Chemistry and Technology 43 (2021) 145–154. 3. Dau D.H., Tung L.M., Hai T.H, Ngoan L.V. - Synthesis of Fe3O4 superparamagnetic nanoparticles and coating process on Fe3O4 nanoparticles, Journal of Science 19a (2011) 38–46. 4. Zhang S., Zhao X., Niu H., Shi Y., Cai Y., Jiang G. - Superparamagnetic Fe3O4 nanoparticles as catalysts for the catalytic oxidation of phenolic and aniline compounds, Journal of Hazardous Materials 167 (2009) 560–566. 5. Thomas N., Dionysios D.D., Suresh C.P. - Heterogeneous fenton catalysts: A review of recent advances, Journal of Hazardous Materials 404 (2021) 124082. 6. Wang W., Mao Q., He H., Zhou M. - Fe3O4 nanoparticles as an efficient heterogeneous Fenton catalyst for phenol removal at relatively wide pH values, Water Science and Technology 68 (11) (2013) 2367–2373. 7. Zelmanov G., Semiat R. - Iron (3) oxide-based nanoparticles as catalysts in advanced organic aqueous oxidation, Water Research 42 (2008) 492–498. 8. Qi G.H., Li X.Q., Cao J. - Research on the phenol degradation in microbial fuel cells with Fe3O4-reduced graphene oxide cathodic catalyst, Advanced Materials Research 881-883 (2014) 310–314. 9. Zhao L., Lin Z., Ma X., Dong Y. - Catalytic activity of different iron oxides: Insight from pollutant degradation and hydroxyl radical formation in heterogeneous Fenton- like systems, Chemical Engineering Journal 352 (2018) 343-351. 10. Hassan H., Fatemeh P., Sohaila A. - Carboxylic acid effects on the size and catalytic activity of magnetite nanoparticles, Journal of Colloid and Interface Science 437 (2015) 1-9. 11. Liu J., Zhao Z., Shao P., Cui P. - Activation of peroxymonosulfate with magnetic Fe3O4– MnO2 core–shell nanocomposites for 4-chlorophenol degradation, Chemical Engineering Journal 262 (2015) 854–861. 18
  19. Comparison of catalytic activities of magnetic iron oxides in phenol degradation 12. Wei Y., Han B., Hu X., Lin Y., Wang X., Deng X. - Synthesis of Fe3O4 nanoparticles and their magnetic properties, Procedia Engineering 27 (2012) 632-637. 13. Mufti N., Atma T., Fuad A., Sutadji E. - Synthesis and characterization of black, red and yellow nanoparticles pigments from the iron sand, International Conference on Theoretical and Applied Physics 2013, AIP Conference Proceedings 1617 (2014) 165-169. 14. Ren B., Xu Y., Zhang C., Zhang L., Zhao J., and Liu Z. - Degradation of methylene blue by a heterogeneous Fenton reaction using an octahedron-like, high-graphitization, carbon-doped Fe2O3 catalyst, Journal of the Taiwan Institute of Chemical Engineers 97 (2019) 170-177. TÓM TẮT SO SÁNH HOẠT TÍNH XÚC TÁC CỦA CÁC OXIT SẮT MANG TỪ TÍNH TRONG PHẢN ỨNG PHÂN HỦY PHENOL Bùi Thị Phương Quỳnh, Lê Thị Kim Anh, Trần Nguyễn An Sa* Trường Đại học Công nghiệp Thực phẩm TP.HCM *Email: satna@hufi.edu.vn Các vật liệu mang từ tính trên nền oxit sắt luôn thu hút được sự chú ý lớn trong lĩnh vực xúc tác do chúng có độ hoạt động hóa học cao, nguồn cung cấp rộng, cũng như dễ thu hồi và tái sử dụng. Nội dung chính của nghiên cứu này là khảo sát hoạt tính xúc tác của các loại oxit sắt, được tổng hợp qua hai quy trình khác nhau, trong phản ứng dị thể kiểu Fenton để phân hủy phenol. Dữ liệu phân tích XRD và SEM cho thấy hai loại oxit sắt là Fe3O4 tinh thể và oxit sắt vô định hình kích thước nano đã được tạo thành. Ảnh hưởng của thời gian phản ứng, lượng hydrogen peroxide và lượng chất xúc tác rắn lên hiệu suất loại bỏ phenol đã được khảo sát chi tiết. Kết quả cho thấy vật liệu từ tính Fe3O4 tinh thể (1-5 μm) cho hiệu suất xử lý phenol cao hơn so với vật liệu oxit sắt vô định hình kích thước nano trong cùng điều kiện phản ứng. Tuy nhiên, tốc độ oxy hóa phenol ban đầu nhanh hơn nhiều khi dùng vật liệu xúc tác oxit sắt vô định hình. Hiệu suất loại bỏ phenol hơn 98% (nồng độ ban đầu 200 ppm) đã đạt được với xúc tác Fe3O4 tinh thể sau 60 phút. Vật liệu oxit sắt vô định hình cũng cho hiệu suất tương đồng chỉ sau 15 phút nhưng cần lượng chất xúc tác và lượng hydrogen peroxide cao hơn đáng kể so với xúc tác Fe3O4 tinh thể. Từ khóa: Phản ứng Fenton, phân hủy phenol, oxit sắt, từ tính. 19
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