Bridging the gap between transition metal- and bio-catalysis via aqueous micellar catalysis
Bridging the gap between transition metal- and bio-catalysis via aqueous micellar catalysis
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DOI：
10.1038/s41467-019-09751-4
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发表时间：
2019-05-15
影响因子：
16.6
通讯作者：
Lipshutz, Bruce H.
中科院分区：
文献类型：
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作者：
Cortes-Clerget, Margery;Akporji, Nnamdi;Lipshutz, Bruce H.
以前的研究表明，设计表面活性剂的水溶液能够在合成有机化学中实现各种有价值的转化。由于反应发生在这些特制的纳米反应器的内部疏水核内，并且其中制备的产物通过水在胶束之间进行动态交换，因此存在使用酶来实现次级过程的机会。在此，我们报告，酮的产品，形成通过初始过渡金属催化反应的基础上的Pd，Cu，Rh，Fe和Au，可以随后在同一锅中的酶促还原醇脱氢酶介导的。最值得注意的是发现存在于水中的纳米胶束似乎不仅作为化学和生物催化的介质，而且作为底物，产物和催化剂的储存库，减少非竞争性酶抑制。
Previous studies have shown that aqueous solutions of designer surfactants enable a wide variety of valuable transformations in synthetic organic chemistry. Since reactions take place within the inner hydrophobic cores of these tailor-made nanoreactors, and products made therein are in dynamic exchange between micelles through the water, opportunities exist to use enzymes to effect secondary processes. Herein we report that ketone-containing products, formed via initial transition metal-catalyzed reactions based on Pd, Cu, Rh, Fe and Au, can be followed in the same pot by enzymatic reductions mediated by alcohol dehydrogenases. Most noteworthy is the finding that nanomicelles present in the water appear to function not only as a medium for both chemo- and bio-catalysis, but as a reservoir for substrates, products, and catalysts, decreasing noncompetitive enzyme inhibition.