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Hemoprotein Catalyzed Oxygenations: P450s, UPOs, and Progress toward Scalable Reactions
JACS Au ( IF 8.5 ) Pub Date : 2021-07-26 , DOI: 10.1021/jacsau.1c00251 Gideon Grogan 1
JACS Au ( IF 8.5 ) Pub Date : 2021-07-26 , DOI: 10.1021/jacsau.1c00251 Gideon Grogan 1
Affiliation
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The selective oxygenation of nonactivated carbon atoms is an ongoing synthetic challenge, and biocatalysts, particularly hemoprotein oxygenases, continue to be investigated for their potential, given both their sustainable chemistry credentials and also their superior selectivity. However, issues of stability, activity, and complex reaction requirements often render these biocatalytic oxygenations problematic with respect to scalable industrial processes. A continuing focus on Cytochromes P450 (P450s), which require a reduced nicotinamide cofactor and redox protein partners for electron transport, has now led to better catalysts and processes with a greater understanding of process requirements and limitations for both in vitro and whole-cell systems. However, the discovery and development of unspecific peroxygenases (UPOs) has also recently provided valuable complementary technology to P450-catalyzed reactions. UPOs need only hydrogen peroxide to effect oxygenations but are hampered by their sensitivity to peroxide and also by limited selectivity. In this Perspective, we survey recent developments in the engineering of proteins, cells, and processes for oxygenations by these two groups of hemoproteins and evaluate their potential and relative merits for scalable reactions.
中文翻译：
血蛋白催化氧化：P450、UPO 和可扩展反应的进展
非活性碳原子的选择性氧化是一项持续的合成挑战，鉴于其可持续的化学凭据和卓越的选择性，生物催化剂，特别是血红蛋白加氧酶，继续研究其潜力。然而，稳定性、活性和复杂反应要求的问题常常使这些生物催化氧化在可扩展的工业过程方面存在问题。对细胞色素 P450 (P450s) 的持续关注，需要减少的烟酰胺辅因子和氧化还原蛋白伙伴来进行电子传输，现在已经导致更好的催化剂和工艺，对体外和全细胞系统的工艺要求和限制有了更深入的了解. 然而，非特异性过氧化酶 (UPO) 的发现和开发最近也为 P450 催化反应提供了有价值的补充技术。UPO 只需要过氧化氢来实现氧化作用，但由于它们对过氧化物的敏感性以及有限的选择性而受到阻碍。在这个视角中，我们调查了蛋白质、细胞和这两组血红素蛋白的氧合过程的最新进展，并评估了它们在可扩展反应中的潜力和相对优点。
更新日期：2021-09-27
中文翻译：
血蛋白催化氧化：P450、UPO 和可扩展反应的进展
非活性碳原子的选择性氧化是一项持续的合成挑战，鉴于其可持续的化学凭据和卓越的选择性，生物催化剂，特别是血红蛋白加氧酶，继续研究其潜力。然而，稳定性、活性和复杂反应要求的问题常常使这些生物催化氧化在可扩展的工业过程方面存在问题。对细胞色素 P450 (P450s) 的持续关注，需要减少的烟酰胺辅因子和氧化还原蛋白伙伴来进行电子传输，现在已经导致更好的催化剂和工艺，对体外和全细胞系统的工艺要求和限制有了更深入的了解. 然而，非特异性过氧化酶 (UPO) 的发现和开发最近也为 P450 催化反应提供了有价值的补充技术。UPO 只需要过氧化氢来实现氧化作用，但由于它们对过氧化物的敏感性以及有限的选择性而受到阻碍。在这个视角中，我们调查了蛋白质、细胞和这两组血红素蛋白的氧合过程的最新进展，并评估了它们在可扩展反应中的潜力和相对优点。
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