Immobilized MAS1 Lipase-catalyzed Synthesis of n-3 PUFA-rich Triacylglycerols in Deep Eutectic Solvents.
Immobilized MAS1 Lipase-catalyzed Synthesis of n-3 PUFA-rich Triacylglycerols in Deep Eutectic Solvents.
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DOI：
10.5650/jos.ess20200
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发表时间：
2021-01
影响因子：
1.5
通讯作者：
Xiumei Wang;Xiaoxu Zhao;Xiaoli Qin;Zexin Zhao;Bo Yang;Yonghua Wang
中科院分区：
文献类型：
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作者：
Xiumei Wang;Xiaoxu Zhao;Xiaoli Qin;Zexin Zhao;Bo Yang;Yonghua Wang
富含N-3多不饱和脂肪酸(PUFA)的三酰基甘油(TAG)具有多种有益作用，目前的合成方法仍难以高效、快速地合成。本研究报道了固定化MAS1脂肪酶的脂肪酸专一性及其在天然深共熔溶剂(NADES)体系中通过甘油和n-3PUFA的酯化反应高效合成富含n-3PUFA的TAG。固定化MAS1脂肪酶对戊酸的选择性最高[C10：0，最高特异性常数(1/α)=1]，而对二十二碳六烯酸和二十碳五烯酸的特异性最低(1/α=0.19和0.2)。在氯化胆碱/甘油(CG)体系中，n-3PUFA含量最高(55.8%)，n-3PUFA组成与底物相近。CG体系中TAG含量是无溶剂体系的1.38倍。有趣的是，固定化MAS1脂肪酶在无溶剂和各种NADS体系中没有区域特异性。此外，还对固定化MAS1脂肪酶催化甘油与n-3多不饱和脂肪酸在NADES体系中的酯化反应机理进行了探讨。研究发现，使用NADES作为溶剂可以大大提高TAG的含量，并使产品易于分离。这些结果表明，固定化MAS1脂肪酶是一种很有前途的生物催化剂，可以在NADS体系中通过甘油和n-3多不饱和脂肪酸的酯化反应高效地合成n-3多不饱和脂肪酸TAG。
n-3 polyunsaturated fatty acids (PUFA)-rich triacylglycerols (TAG) with many beneficial effects are still difficult to be synthesized efficiently and rapidly by current synthetic techniques. This study reports the fatty acid specificity of immobilized MAS1 lipase and its efficient synthesis of n-3 PUFA-rich TAG by esterification of glycerol with n-3 PUFA in natural deep eutectic solvents (NADES) systems. Immobilized MAS1 lipase showed the highest preference for capric acid [C10:0, the highest specificity constant (1/α)=1] whereas it discriminated strongly against docosahexaenoic acid (DHA) and eicosapentaenoic acid (EPA) due to their lowest specificity constants (1/α=0.19 and 0.2). Moreover, the highest n-3 PUFA-rich TAG content (55.8%) with similar n-3 PUFA composition to the substrate was obtained in choline chloride/glycerol (CG) system. There was a 1.38-fold increase of TAG content in CG system compared with that in the solvent-free system. Interestingly, immobilized MAS1 lipase exhibited no regiospecificity in the solvent-free and various NADES systems. Besides, the potential reaction mechanism of immobilized MAS1 lipase-catalyzed esterification of glycerol with n-3 PUFA in NADES systems was described. It was found that the use of NADES as solvents could greatly enhance TAG content, and make it easy to separate the product. These results indicated that immobilized MAS1 lipase is a promising biocatalyst for the efficient synthesis of n-3 PUFA-rich TAG by esterification of glycerol with n-3 PUFA in NADES systems.