Engineering Spatially Organized Multienzyme Assemblies for Complex Chemical Transformation
Engineering Spatially Organized Multienzyme Assemblies for Complex Chemical Transformation
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DOI：
10.1021/acscatal.8b01883
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发表时间：
2018-09-01
期刊：
影响因子：
12.9
通讯作者：
Wen, Fei
中科院分区：
文献类型：
--
作者：
Bugada, Luke F.;Smith, Mason R.;Wen, Fei
在过去的二十年中，酶催化已经成为传统催化的经济和环境友好的替代品，在制药，1食品，2和化妆品3行业中有许多应用。在它们的优点中，许多酶表现出比它们的金属对应物显著更大的活性、对映选择性和特异性，4提高了过程效率并增加了产物产率。此外，酶往往在相对温和的温度和压力下表现出最佳活性，减少能量消耗，从而降低操作成本。大多数工业酶用于单步反应;然而，通过使用多种酶催化复杂的化学转化，可以大大扩展酶催化的潜在应用。复杂的化学转化涉及两个或多个酶催化反应，它们通过顺序、耦合、发散和/或收敛反应步骤5 - 7相互关联（图1）。复杂的化学转化在从蛋白质合成到细胞代谢的生物过程中是常见的。在自然界中，微生物已经进化出通过共定位功能相关的酶来最大化某些复杂化学转化的催化效率的特征。8 - 11近年来，研究人员从天然酶的共定位中获得灵感，并应用蛋白质工程的进展来创造新的多酶组装体（MEA），对参与酶的分子比例和空间组织进行非凡的控制。已经采用了几种策略来实现对这些参数的控制，包括DNA支架、12种蛋白质支架、13种基于聚合物颗粒的组装体、14种金属有机框架、15种交联酶聚集体。16.虽然多边环境协定在结构和机理上各不相同，但其最终目标是加快反应速度和提高反应效率，我们认为，多边环境协定将成为在各种领域生产复杂分子的传统催化方法的一种越来越有吸引力的替代方法。在这里，我们强调了MEA工程的有前途的进展，并总结了这些系统在商业生产过程中必须克服的技术挑战。
Over the past two decades, enzyme catalysis has emerged as an economical and environmentally friendly alternative to conventional catalysis with numerous applications in the pharmaceutical, 1 food, 2 and cosmetic 3 industries. Among their advantages, many enzymes exhibit significantly greater activity, enantioselectivity, and specificity than their metal counterparts, 4 improving process efficiency and increasing product yields. In addition, enzymes tend to exhibit optimal activities at relatively mild temperatures and pressures, reducing energy consumption and thereby lowering operating costs. The majority of industrial enzymes are used in singlestep reactions; however, the potential applications of enzyme catalysis can be greatly expanded by using multiple enzymes to catalyze complex chemical transformations. Complex chemical transformations involve two or more enzyme-catalyzed reactions, which are related through sequential, coupled, divergent, and/or convergent reaction steps 5− 7 (Figure 1). Complex chemical transformations are common in biological processes ranging from protein synthesis to cellular metabolism. In nature, microorganisms have evolved features to maximize the catalytic efficiency of some complex chemical transformations by colocalizing functionally related enzymes. 8− 11 In recent years, researchers have drawn inspiration from natural enzyme colocalization and applied advances in protein engineering to create novel multienzyme assemblies (MEAs) that provide extraordinary control over the molecular ratio and spatial organization of the participating enzymes. Several strategies have been employed to achieve control over these parameters including DNA scaffolds, 12 protein scaffolds, 13 polymeric particle-based assemblies, 14 metal− organic frameworks, 15 and cross-linked enzyme aggre-gates. 16 While structurally and mechanistically diverse, the ultimate goal of MEAs is to accelerate reaction rates and increase reaction efficiency.In our view, MEAs will become an increasingly attractive alternative to conventional catalytic processes for the production of complex molecules in a variety of fields. Here we highlight promising advances in MEA engineering and summarize technical challenges that must be overcome for these systems to be used in commercial production processes.