Kudalkar Gaurav P, Tiwari Virendra K, Berkowitz David B
Department of Chemistry, University of Nebraska, Lincoln, Nebraska 68588-0304 USA.
ChemCatChem. 2024 Nov 11;16(21). doi: 10.1002/cctc.202400835. Epub 2024 Jul 8.
Billions of years of evolution have led to the selection of (hyper)thermophiles capable of flourishing at elevated temperatures. The corresponding native (hyper)thermophilic enzymes retain their tertiary and quaternary structures at near-boiling water temperatures and naturally retain catalytically competent conformational dynamics under these conditions. And yet, while hyper/thermophilic enzymes offer special opportunities in biocatalysis and in hybrid bio/chemocatalytic approaches to modern synthesis in both academia and industry, these enzymes remain underexplored in biocatalysis. Among the strategic advantages that can be leveraged in running biocatalytic transformations at higher temperatures are included more favorable kinetics, removal of volatile byproducts to drive reactions forward, improved substrate solubility and product separation, and accelerated stereodynamics for dynamic kinetic resolutions. These topics are discussed and illustrated with contemporary examples of note, in sections organized by stratagem. Finally, the reader is alerted in particular to archaeal enzymes that have proven useful in non-natural synthetic chemistry ventures, and at the same time is referred to a rich area of archaea whose genomes have been sequenced but whose enzymatic activities of interest have not yet been mined. Though hyperthermophilic archaea are among the most ancient of organisms, their enzymes may hold the key to many future innovations in biocatalytic chemistry - perhaps we really do need to go 'back to the future'.
数十亿年的进化导致了能够在高温下蓬勃生长的(超)嗜热菌的出现。相应的天然(超)嗜热酶在接近沸水的温度下保持其三级和四级结构,并在这些条件下自然地保持具有催化活性的构象动力学。然而,尽管超嗜热酶在学术界和工业界的生物催化以及现代合成的生物/化学催化混合方法中提供了特殊机会,但这些酶在生物催化领域仍未得到充分探索。在较高温度下进行生物催化转化可以利用的战略优势包括更有利的动力学、去除挥发性副产物以推动反应进行、提高底物溶解度和产物分离效果,以及加速动态动力学拆分的立体动力学。这些主题将在按策略组织的章节中通过当代的显著例子进行讨论和说明。最后,特别提醒读者注意已证明在非天然合成化学项目中有用的古菌酶,同时指出古菌的一个丰富领域,其基因组已被测序,但其感兴趣的酶活性尚未被挖掘。尽管超嗜热古菌是最古老的生物之一,但其酶可能是生物催化化学未来许多创新的关键——也许我们真的需要“回到未来”。