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The nature of chemical innovation: new enzymes by evolution
Quarterly Reviews of Biophysics ( IF 6.1 ) Pub Date : 2015-11-05 , DOI: 10.1017/s003358351500013x Frances H Arnold 1
Quarterly Reviews of Biophysics ( IF 6.1 ) Pub Date : 2015-11-05 , DOI: 10.1017/s003358351500013x Frances H Arnold 1
Affiliation
I describe how we direct the evolution of non-natural enzyme activities, using chemical intuition and information on structure and mechanism to guide us to the most promising reaction/enzyme systems. With synthetic reagents to generate new reactive intermediates and just a few amino acid substitutions to tune the active site, a cytochrome P450 can catalyze a variety of carbene and nitrene transfer reactions. The cyclopropanation, N–H insertion, C–H amination, sulfimidation, and aziridination reactions now demonstrated are all well known in chemical catalysis but have no counterparts in nature. The new enzymes are fully genetically encoded, assemble and function inside of cells, and can be optimized for different substrates, activities, and selectivities. We are learning how to use nature's innovation mechanisms to marry some of the synthetic chemists’ favorite transformations with the exquisite selectivity and tunability of enzymes.
中文翻译:
化学创新的本质:进化中的新酶
我描述了我们如何指导非天然酶活性的进化,使用化学直觉和有关结构和机制的信息来指导我们找到最有前途的反应/酶系统。使用合成试剂生成新的反应性中间体,只需几个氨基酸取代即可调节活性位点,细胞色素 P450 可以催化各种卡宾和氮烯转移反应。现在证明的环丙烷化、N-H 插入、C-H 胺化、亚磺酰亚胺化和氮丙啶化反应在化学催化中都是众所周知的,但在自然界中没有对应物。新酶在细胞内完全基因编码、组装和发挥作用,并且可以针对不同的底物、活性和选择性进行优化。我们正在学习如何利用自然'
更新日期:2015-11-05
中文翻译:
化学创新的本质:进化中的新酶
我描述了我们如何指导非天然酶活性的进化,使用化学直觉和有关结构和机制的信息来指导我们找到最有前途的反应/酶系统。使用合成试剂生成新的反应性中间体,只需几个氨基酸取代即可调节活性位点,细胞色素 P450 可以催化各种卡宾和氮烯转移反应。现在证明的环丙烷化、N-H 插入、C-H 胺化、亚磺酰亚胺化和氮丙啶化反应在化学催化中都是众所周知的,但在自然界中没有对应物。新酶在细胞内完全基因编码、组装和发挥作用,并且可以针对不同的底物、活性和选择性进行优化。我们正在学习如何利用自然'