Better than Nature: Nicotinamide Biomimetics That Outperform Natural Coenzymes.
Better than Nature: Nicotinamide Biomimetics That Outperform Natural Coenzymes.
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DOI：
10.1021/jacs.5b12252
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发表时间：
2016-01-27
影响因子：
15
通讯作者：
Scrutton NS
中科院分区：
文献类型：
--
作者：
Knaus T;Paul CE;Levy CW;de Vries S;Mutti FG;Hollmann F;Scrutton NS
寻找经济实惠的绿色生物催化工艺是化学品生产的一个挑战。氧化还原生物转化具有潜在的吸引力，但它们依赖于不稳定且昂贵的烟酰胺辅酶，这阻碍了它们的广泛利用。天然辅酶的化学计量使用在经济上是不可行的，并且这些分子的不稳定性阻碍了采用辅酶再循环的催化过程。在这里，我们研究了天然辅酶NAD（P）H的人工合成仿生在氧化还原生物催化中的效率。对属于“烯”还原酶家族的一系列氧化还原酶的广泛研究表明，这些仿生物是天然辅酶的优异类似物，也在具有所选仿生物的烯还原酶XenA的晶体结构中揭示。在某些情况下，这些仿生学优于天然辅酶。通过利用高立体、区域和化学选择性氧化还原生物催化剂的力量，并在温和条件下以低成本实现反应，“优于自然”的仿生学应该在精细和特种化学品生产中得到广泛应用。
The search for affordable, green biocatalytic processes is a challenge for chemicals manufacture. Redox biotransformations are potentially attractive, but they rely on unstable and expensive nicotinamide coenzymes that have prevented their widespread exploitation. Stoichiometric use of natural coenzymes is not viable economically, and the instability of these molecules hinders catalytic processes that employ coenzyme recycling. Here, we investigate the efficiency of man-made synthetic biomimetics of the natural coenzymes NAD(P)H in redox biocatalysis. Extensive studies with a range of oxidoreductases belonging to the “ene” reductase family show that these biomimetics are excellent analogues of the natural coenzymes, revealed also in crystal structures of the ene reductase XenA with selected biomimetics. In selected cases, these biomimetics outperform the natural coenzymes. “Better-than-Nature” biomimetics should find widespread application in fine and specialty chemicals production by harnessing the power of high stereo-, regio-, and chemoselective redox biocatalysts and enabling reactions under mild conditions at low cost.