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内分子C-H键氨基化,由与铁甲复制的肌红蛋白催化

Yoshiyuki Kagawa¹, Koji Oohora², Takashi Hayashi¹

¹Department of Applied Chemistry, Graduate School of Engineering, Osaka University, Suita, Osaka, 565-0871, Japan.

Journal of inorganic biochemistry

|January 5, 2024

概括

用铁烯 (rMb(FePc)) 溶解的肌球蛋白有效催化C-H键氨基化反应. 这种人工酶系统显示了提高生产含化合物的效率和选择性.

科学领域:

生物化学生物化学
有机化学有机化学
催化剂是一种催化剂.

背景情况:

C-H 键氨基化对于合成含分子至关重要.
肌球蛋白是一种天然蛋白质,具有潜在的催化应用.
开发用于C-H功能化的高效催化剂仍然是一个重大挑战.

研究的目的:

为了研究与铁烯 (rMb(FePc)) 溶解的肌球蛋白的催化活性,用于分子内C-H键氨基化.
在这个反应中,将rMb(FePc) 与原生髓质蛋白的性能进行比较.
探索特定突变对rMb(FePc的催化效率和选择性的影响.

主要方法:

肌球蛋白与铁 (FePc) 的复合,形成rMb(FePc).
催化试验用于亚利硫尼尔亚化物的分子内C-H键氨基化.
动力学研究以确定催化参数 (kcat).
肌球蛋白 (H64A,H64V,H64I) 的位点定向突变发生和突变的rMb(FePc) 酶的表征.

主要成果:

rMb(FePc) 能够成功地催化烯硫酸的分子内C(sp3) -H键氨基化,形成酸类似物.
rMb(FePc) 在特定基板上实现了高达5.7×104的总营业额 ().
rMb(FePc) 与原生肌球蛋白相比,对氨基化对亚化降解的选择性更高.
动力学分析显示,rMb{\displaystyle rMb{\displaystyle rMb}{\displaystyle rFeP}{\displaystyle rMb}{\displaystyle rFeP}{\displaystyle rMb}{\displaystyle rFeP}{\displaystyle rMb}{\displaystyle rFeP}{\displaystyle rMb}{\displaystyle rMb}{\displaystyle rFeP}{\displaystyle rMb}{\displaystyle rFeP}{\displaystyle rMb}{\displaystyle rFeP}{\displaystyle rMb}{\displaystyle rMb}{\displaystyle rFeP}{\displaystyle rFeP}{\displaystyle rMb{\displaystyle rMb}{\displaystyle rFeP}{\displaystyle rMb{\displaystyle rFeP}}) 的基因比原生肌球蛋白高出4倍.
突变的rMb(FePc) 变种 (H64A,H64V,H64I) 表现出增强的TON和反选择性.

结论:

铁素作为有效的人工辅助因子为肌球蛋白在催化C-H键氨基化.
rMb(FePc) 提供了改善的催化效率和选择性,用于sultanam合成.
通过特定突变对肌球蛋白的蛋白质工程可以进一步优化催化性能.

关键词:

人工金属酶是一种人工金属酶.CH键的功能化功能化铁甲是一种铁甲.骨髓蛋白质是什么骨髓蛋白质是什么亚转移转移的亚.苏尔塔姆合成的方法

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