大目金枪鱼加工副产物中鱼油提取制备及EPA分离纯化
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摘要
为获得较高纯度的乙酯型EPA金枪鱼油,以大目金枪鱼加工副产物为原料,通过响应面法优化酶辅助提取粗鱼油的工艺参数,并采用粗鱼油精制、化学催化乙酯化、多级分子蒸馏和尿素包合初步纯化、精馏高纯化,以及合成银离子功能材料螯合制备分离等一系列技术手段进行制备。结果表明,优化的酶解提取法工艺条件为:酶解pH值8.5、酶解温度45℃、酶解时间3 h,此条件下粗鱼油提取率高达43.69%。乙酯化鱼油经多级分子蒸馏和尿素包合处理后,EPA和DHA总量可达80.00%以上,且分别占46.34%和34.58%。对该鱼油进行精馏试验,获得EPA乙酯,其含量达到82.40%,得率为39.00%,在此基础上,进一步使用银硫醇硅胶制备得到96.30%的EPA乙酯,得率为32.90%。本研究结果为鱼类加工副产物的高值化利用提供了一定参考。
In this study, the processed by-products of tuna(T. obesus) was used as the major raw material for preparative separation of fish oil with high content of ethyl type EPA tuna oil by a series of technologies, including optimized extraction of enzyme-assisted extraction of crude fish oil, refinement, chemical ethyl esterification, molecular distillation and urea complexation for preliminary purification, rectification, and silver functionalized material based on separation. The optimal extraction parameters of crude fish oil were as follows: pH was 8.5, enzyme temperature was 45℃, and time was 3 h, and the yield of crude fish oil reached 43.69% under the optimal conditions. The total content of EPA and DHA in purified fish oil was over 80.00%, and the content of EPA and DHA reached 46.34% and 34.58% respectively after being treated by multi-stage molecular distillation and urea complexation treatment. In order to obtain pure EPA ethyl ester, the fish oil was further rectified and the content of EPA ethyl ester reached 82.40% with yield 39.00%. After the preparative separation by silver functionalized material chelating, the content of EPA ethyl ester reached 96.30% with yield 32.90%. This study provides references for the high value utilization of fish processed by-products.
In this study, the processed by-products of tuna(T. obesus) was used as the major raw material for preparative separation of fish oil with high content of ethyl type EPA tuna oil by a series of technologies, including optimized extraction of enzyme-assisted extraction of crude fish oil, refinement, chemical ethyl esterification, molecular distillation and urea complexation for preliminary purification, rectification, and silver functionalized material based on separation. The optimal extraction parameters of crude fish oil were as follows: pH was 8.5, enzyme temperature was 45℃, and time was 3 h, and the yield of crude fish oil reached 43.69% under the optimal conditions. The total content of EPA and DHA in purified fish oil was over 80.00%, and the content of EPA and DHA reached 46.34% and 34.58% respectively after being treated by multi-stage molecular distillation and urea complexation treatment. In order to obtain pure EPA ethyl ester, the fish oil was further rectified and the content of EPA ethyl ester reached 82.40% with yield 39.00%. After the preparative separation by silver functionalized material chelating, the content of EPA ethyl ester reached 96.30% with yield 32.90%. This study provides references for the high value utilization of fish processed by-products.
引文
[1] Yukitaka S, Toshiyuki Y, Toshio Ⅰ, Kazuki M, Kinya K. Detection of bluefin tuna blood flukes (Cardicola spp.) from wild juvenile Pacific bluefin tuna Thunnus orientalis caught for aquaculture[J]. Aquaculture, 2016, 452(2):9-11
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[4] 沈清, 金仁耀, 冯俊丽, 薛静, 陈康, 戴志远. 二醇基硅胶固相萃取-多维质谱对乌鳢组织脂质组学研究[J]. 食品科学, 2017, 38(2): 154-158
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[7] 崔益玮, 俞喜娜, 李诗言, 戴志远, 陈康, 沈清. 直接进样串联质谱法快速筛查水产副产物中ω-3脂肪酸链磷脂[J]. 食品科学, 2018, 97(8): 97-102
[8] 张蒙娜, 宋恭帅, 彭茜, 薛静, 朱凤仙, 戴志远. 响应面法优化精制沙丁鱼EPA和DHA富集工艺[J]. 中国油脂, 2018, 43(8):42-46
[9] Shen Q, Wang Y, Gong L, Guo R, Dong W, Cheung H. Shotgun lipidomics strategy for fast analysis of phospholipids in fisheries waste and its potential in species differentiation[J]. Journal of Agricultural and Food Chemistry, 2012, 60(37): 9384-9393
[10] 林文, 田龙, 王志祥, 杜起光. 尿素包合法联合分子蒸馏技术提纯乙酯化鱼油中EPA及DHA的工艺研究[J]. 中国粮油学报, 2012, 27(12): 84-88
[11] 张良, 刘美玲, 董强, 刘书成, 郝记明, 张静. 硝酸银硅胶柱分离纯化蛇鲻鱼油中的EPA和DHA[J]. 中国粮油学报, 2011, 26(12):63-68
[12] 王芳. 淡水鱼鱼油的制备及微胶囊化研究[D]. 武汉: 华中农业大学, 2009: 15-20
[13] Sahena F, Ism Z, Jinap S, Yazid A, Khatib A, Nan N. Fatty acid compositions of fish oil extracted from different parts of Indian mackerel (Rastrelliger kanagurta) using various techniques of supercritical CO2, extraction[J]. Food Chemistry, 2010, 120(3): 879-885
[14] 徐华, 张茹, 刘连亮, 张进杰, 杨文鸽, 楼乔明. 辣木籽油脂微波提取工艺优化及其脂质分析[J]. 核农学报, 2018, 32(7): 1393-1399
[15] 李云松, 杨同舟, 徐宏军. 鱼油中EPA和DHA的富集研究新进展[J]. 西部粮油科技, 2002, 27(5): 27-30
[16] Crexi Ⅴ, Monte M, Soares L, Pinto L. Production and refinement of oil from carp (Cyprinus carpio) viscera[J]. Food Chemistry, 2010, 119(1): 945-950
[17] 张旭冬, 胡志雄, 张维农, 贺军波, 齐玉堂. 巯基键合银离子色谱固定相的制备及其在油脂分析中的应用[J]. 食品安全质量检测学报, 2016, 7(4): 1607-1612
[18] Shen Q, Guo R, Dai Z, Zhang Y. Investigation of enzymatic hydrolysis conditions on the properties of protein hydrolysate from fish muscle (Collichthys niveatus) and evaluation of its functional properties[J]. Journal of Agricultural and Food Chemistry, 2012, 60(20): 5192-5198
[19] 吴奎元. 酶解带鱼内脏提取鱼油及防止其氧化研究[D]. 福州: 福建农林大学, 2011: 21-25
[20] 王佳莉. 蛋白酶水解金枪鱼副产物的工艺研究[D]. 广州: 华南理工大学, 2011: 31-33
[21] 洪毅敏, 马金萍, 张艳纹, 陈月英, 许新德, 章鹏飞. 气相色谱法测定乙酯型鱼油微胶囊产品中EPA乙酯和DHA乙酯含量[J]. 中国油脂, 2015, 40(12): 88-91
[22] 傅红, 裘爱泳. 鱼油质构脂质的高温气相色谱分析[J]. 中国粮油学报, 2005, 20(4): 101-104
[23] Fala L. Vascepa: first EPA only omega-3 therapy approved by the FDA for severe hypertriglyceridemia[J]. American Health & Drug Benefits, 2013, 1(4): 252
[24] 汤小会. 竹荚鱼加工废弃物中鱼油的分离提取[J]. 食品工业科技, 2009, 30(5): 251-252
[25] 陶轶, 吴芮, 包建强. 甲鱼油的主要成分及提取方法的研究进展[J]. 中国油脂, 2015, 40(8): 74-76
[26] Carvajal A, Slizyte R, Storr? Ⅰ, Aursand M. Production of high quality fish oil by enzymatic protein hydrolysis from cultured Atlantic salmon by-products: Investigation on effect of various extraction parameters using central composite rotatable design[J]. Waste & Biomass Valorization, 2017, 9(11): 1-12
[27] 周绪霞, 陈红, 陈婷, 吕飞, 顾赛麒, 丁玉庭. 脂质对食品中蛋白质凝胶特性的影响及其作用机制[J]. 核农学报, 2018, 32(9): 1808-1813
[28] 陶宁萍, 周敏, 王锡昌. 提取黄鳍金枪鱼眼窝肉鱼油的方法比较研究[J]. 中国油脂, 2011, 36(1): 41-44
[29] 傅红, 裘爱泳. 分子蒸馏法富集鱼油ω-3脂肪酸[J]. 中国粮油学报, 2006, 21(3): 156-159
[30] 田龙, 林文, 王志祥, 赵思昆, 王萍. 深海鱼油中EPA和DHA的富集方法研究进展[J]. 药物生物技术, 2008, 15(6): 489-492
[31] Beaudoin L, Gevariya N, Robitaille K, Guertin M, Pelletier J, Julien P, Fradet Ⅴ. PD42-09 effects of omega-3-rich fish oil (mag-EPA) on prostate cancer: preliminary results of a clinical trial[J]. Journal of Urology, 2018, 199(4): 817-818
[2] 李明爽. 全球金枪鱼产量增加但过度捕捞仍持续[J]. 中国水产, 2016(10): 78-78
[3] Jin R, Li L, Feng J, Dai Z, Huang Y, Shen Q. Zwitterionic hydrophilic interaction solid-phase extraction and multi-dimensional mass spectrometry for shotgun lipidomic study of hypophthalmichthys nobilis[J]. Food Chemistry, 2017, 216(2): 347-354
[4] 沈清, 金仁耀, 冯俊丽, 薛静, 陈康, 戴志远. 二醇基硅胶固相萃取-多维质谱对乌鳢组织脂质组学研究[J]. 食品科学, 2017, 38(2): 154-158
[5] 崔益玮, 李诗言, 王珏, 宋恭帅, 王扬, 戴志远, 沈清. 水产副产物中磷脂和鱼油的分离及脂质组学研究[J]. 水产学报, 2017, 41(6): 827-835
[6] Shen Q, Cheung H. A TiO2/SiO2 core-shell composites based sample preparation method for selective extraction of phospholipids from shrimp waste followed by HILIC-QTOF/MS analysis[J]. Journal of Agricultural and Food Chemistry, 2014, 62(36): 8944-8951
[7] 崔益玮, 俞喜娜, 李诗言, 戴志远, 陈康, 沈清. 直接进样串联质谱法快速筛查水产副产物中ω-3脂肪酸链磷脂[J]. 食品科学, 2018, 97(8): 97-102
[8] 张蒙娜, 宋恭帅, 彭茜, 薛静, 朱凤仙, 戴志远. 响应面法优化精制沙丁鱼EPA和DHA富集工艺[J]. 中国油脂, 2018, 43(8):42-46
[9] Shen Q, Wang Y, Gong L, Guo R, Dong W, Cheung H. Shotgun lipidomics strategy for fast analysis of phospholipids in fisheries waste and its potential in species differentiation[J]. Journal of Agricultural and Food Chemistry, 2012, 60(37): 9384-9393
[10] 林文, 田龙, 王志祥, 杜起光. 尿素包合法联合分子蒸馏技术提纯乙酯化鱼油中EPA及DHA的工艺研究[J]. 中国粮油学报, 2012, 27(12): 84-88
[11] 张良, 刘美玲, 董强, 刘书成, 郝记明, 张静. 硝酸银硅胶柱分离纯化蛇鲻鱼油中的EPA和DHA[J]. 中国粮油学报, 2011, 26(12):63-68
[12] 王芳. 淡水鱼鱼油的制备及微胶囊化研究[D]. 武汉: 华中农业大学, 2009: 15-20
[13] Sahena F, Ism Z, Jinap S, Yazid A, Khatib A, Nan N. Fatty acid compositions of fish oil extracted from different parts of Indian mackerel (Rastrelliger kanagurta) using various techniques of supercritical CO2, extraction[J]. Food Chemistry, 2010, 120(3): 879-885
[14] 徐华, 张茹, 刘连亮, 张进杰, 杨文鸽, 楼乔明. 辣木籽油脂微波提取工艺优化及其脂质分析[J]. 核农学报, 2018, 32(7): 1393-1399
[15] 李云松, 杨同舟, 徐宏军. 鱼油中EPA和DHA的富集研究新进展[J]. 西部粮油科技, 2002, 27(5): 27-30
[16] Crexi Ⅴ, Monte M, Soares L, Pinto L. Production and refinement of oil from carp (Cyprinus carpio) viscera[J]. Food Chemistry, 2010, 119(1): 945-950
[17] 张旭冬, 胡志雄, 张维农, 贺军波, 齐玉堂. 巯基键合银离子色谱固定相的制备及其在油脂分析中的应用[J]. 食品安全质量检测学报, 2016, 7(4): 1607-1612
[18] Shen Q, Guo R, Dai Z, Zhang Y. Investigation of enzymatic hydrolysis conditions on the properties of protein hydrolysate from fish muscle (Collichthys niveatus) and evaluation of its functional properties[J]. Journal of Agricultural and Food Chemistry, 2012, 60(20): 5192-5198
[19] 吴奎元. 酶解带鱼内脏提取鱼油及防止其氧化研究[D]. 福州: 福建农林大学, 2011: 21-25
[20] 王佳莉. 蛋白酶水解金枪鱼副产物的工艺研究[D]. 广州: 华南理工大学, 2011: 31-33
[21] 洪毅敏, 马金萍, 张艳纹, 陈月英, 许新德, 章鹏飞. 气相色谱法测定乙酯型鱼油微胶囊产品中EPA乙酯和DHA乙酯含量[J]. 中国油脂, 2015, 40(12): 88-91
[22] 傅红, 裘爱泳. 鱼油质构脂质的高温气相色谱分析[J]. 中国粮油学报, 2005, 20(4): 101-104
[23] Fala L. Vascepa: first EPA only omega-3 therapy approved by the FDA for severe hypertriglyceridemia[J]. American Health & Drug Benefits, 2013, 1(4): 252
[24] 汤小会. 竹荚鱼加工废弃物中鱼油的分离提取[J]. 食品工业科技, 2009, 30(5): 251-252
[25] 陶轶, 吴芮, 包建强. 甲鱼油的主要成分及提取方法的研究进展[J]. 中国油脂, 2015, 40(8): 74-76
[26] Carvajal A, Slizyte R, Storr? Ⅰ, Aursand M. Production of high quality fish oil by enzymatic protein hydrolysis from cultured Atlantic salmon by-products: Investigation on effect of various extraction parameters using central composite rotatable design[J]. Waste & Biomass Valorization, 2017, 9(11): 1-12
[27] 周绪霞, 陈红, 陈婷, 吕飞, 顾赛麒, 丁玉庭. 脂质对食品中蛋白质凝胶特性的影响及其作用机制[J]. 核农学报, 2018, 32(9): 1808-1813
[28] 陶宁萍, 周敏, 王锡昌. 提取黄鳍金枪鱼眼窝肉鱼油的方法比较研究[J]. 中国油脂, 2011, 36(1): 41-44
[29] 傅红, 裘爱泳. 分子蒸馏法富集鱼油ω-3脂肪酸[J]. 中国粮油学报, 2006, 21(3): 156-159
[30] 田龙, 林文, 王志祥, 赵思昆, 王萍. 深海鱼油中EPA和DHA的富集方法研究进展[J]. 药物生物技术, 2008, 15(6): 489-492
[31] Beaudoin L, Gevariya N, Robitaille K, Guertin M, Pelletier J, Julien P, Fradet Ⅴ. PD42-09 effects of omega-3-rich fish oil (mag-EPA) on prostate cancer: preliminary results of a clinical trial[J]. Journal of Urology, 2018, 199(4): 817-818