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Membrane-supported aqueous-phase enzymatic conversions in organic solvents.

机译:有机溶剂中膜支持的水相酶促转化。

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A new concept membrane immobilized enzyme bioreactor is developed. Enzyme is placed in a thin film of water strongly associated with the inner surface of a hydrophilic microporous membrane and is either adsorbed on the membrane or freely dissolved in an aqueous phase. Substrate dissolved in a water-immiscible organic solvent is convectively permeated through the membrane and converted into product by the enzyme reaction. The permeation flux is controlled by transmembrane pressure, therefore, efficient mass transfer with continuous operation is achieved.; This concept was tested using tyrosinase-catalyzed oxidation of p-cresol in chloroform and the effects of the operating parameters on performance were studied. The initial reaction rate quickly decreased and was followed by relatively stable period. The experimental results showed that the initial activity loss was due to enzyme transport in both axial and radial directions. Approaches to reduce the movement of enzyme and to improve activity are suggested. Water content and permeation flux were the most important parameters effecting performance for the system.; A mathematical model describing the behavior of the system was developed using experimentally determined parameters. By separating the effect of water content and permeation flux on the enzyme activity, the optimal operating conditions could be determined.; Also, alcohol dehydrogenase-catalyzed oxidoreduction of alcohol and aldehyde was employed to test the applicability of the technique. It appears that the membrane supported aqueous-phase enzyme reactor is also useful with enzymes requiring cofactors.; The experimental results using two model enzyme-catalyzed reactions indicate that although the initial decrease of activity remained a problem, membrane supported aqueous-phase is a useful technique with enormous potential for enzyme-catalyzed reactions.
机译:开发了一种新概念的膜固定酶生物反应器。酶被置于与亲水性微孔膜的内表面紧密结合的水薄膜中,或者被吸附在膜上,或者被自由地溶解在水相中。溶于水不混溶的有机溶剂中的底物通过膜对流渗透,并通过酶反应转化为产物。渗透通量是由跨膜压力控制的,因此,可以实现连续操作的有效传质。使用酪氨酸酶催化的对甲酚在氯仿中的氧化测试了该概念,并研究了操作参数对性能的影响。最初的反应速率迅速降低,随后是相对稳定的时期。实验结果表明,初始活性损失是由于酶在轴向和径向方向上的运输。提出了减少酶运动并提高活性的方法。水分和渗透通量是影响系统性能的最重要参数。使用实验确定的参数开发了描述系统行为的数学模型。通过分离水分含量和渗透通量对酶活性的影响,可以确定最佳的操作条件。同样,采用醇脱氢酶催化的醇和醛的氧化还原来测试该技术的适用性。似乎膜支持的水相酶反应器也可用于需要辅因子的酶。使用两个模型酶催化反应的实验结果表明,尽管活性的初始下降仍然是一个问题,但膜负载水相是一种有用的技术,具有巨大的酶催化潜力。

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