通过阿齐多集团的协助,重新利用非海姆铁氧化酶以实现催化的安装
Madison Davidson1, Meredith McNamee1, Ruixi Fan2
1Department of Chemistry , North Carolina State University , Raleigh , North Carolina 27695 , United States.
Journal of the American Chemical Society
|February 14, 2019
概括
铁酶可以通过引入一个基组来重定向形成基而不是基. 这一发现扩大了非血铁和2-酸依赖酶的催化能力.
科学领域:
- 生物化学
- 酵素学
- 有机化学
背景情况:
- 非海姆铁和2-氧格酸盐 (Fe/2OG) 依赖的酶催化化反应.
- 此前已发现的酶包括l-Ile 4-基酶,l-Leu 5-基酶和多二基酶.
研究的目的:
- 为了研究Fe/2OG基酶与白异构体的基质范围.
- 通过基质改性来证明Fe/2OG酶的催化活性的重定向.
- 探索除了正规化之外的新型酶变化.
主要方法:
- 使用白同位素和改性基质的酶分析.
- 反应产品的表征以确定区域特异性和识别新变化.
- 涉及C-H键激活和酸组定向酸形成的机制研究.
主要成果:
- 铁/2OG氧化酶容纳白同位素,催化特定区域的氧化.
- 引入一个亚基将酶重定向到安装一个基基而不是基基.
- 反应通过Fe (IV) -oxo物种的C-H键激活,然后由酸导向的CN键形成.
结论:
- /2OG酶具有比以前更广泛的基质接受和催化多功能性.
- 基质辅助工程可以重定向Fe/2OG酶以执行非原生反应,如化物安装.
- 这项研究为扩大Fe/2OG酶的合成范围开辟了新的途径.
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