铁酶的H与化物之间的相互作用
Melisa Del Barrio1, Matteo Sensi1, Laura Fradale1
1Aix Marseille Université , CNRS, Bioénergétique et Ingénierie des Protéines , Marseille , France.
Journal of the American Chemical Society
|March 29, 2018
概括
在氧化条件下FeFe酶被反向无活化,但只有当或离子存在时. 这些化物与催化中间体结合,导致稳定,不活跃的酶状态.
科学领域:
- 生物化学
- 酵素学
- 生物有机化学
背景情况:
- FeFe酶是H2代谢的关键酶.
- 在特定的条件下,酶的可逆失活性尚不清楚.
- 之前的假设涉及ADT连接或非生产性H2连接.
研究的目的:
- 阐明FeFe酶无氧,氧化,H2依赖性失活的机制.
- 研究化物在酶失活中的作用.
- 为抑制酶状态提出结构模型.
主要方法:
- 酶动力学研究以确定抑制类型.
- 密度功能理论 (DFT) 计算以建模酶结构.
- 进行光谱检测 (建议).
主要成果:
- 无活化完全取决于Cl-或Br-的存在.
- 作为一种非竞争性抑制剂,与催化中间体结合.
- 在化物结合时,氧化会将酶锁定到稳定不活的形式.
- 化物与adt连接体的氨基组相互作用,而不是直接与铁相互作用.
结论:
- 之前提出的禁用机制是不够的.
- 化物离子在FeFe酶的可逆失活中起着关键作用.
- 提出了一种涉及化物与催化中间体结合的新机制.
- 这些发现为进一步研究稳定抑制状态开辟了道路.
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