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单分子驱动的纳米马达揭示了活性酶的动态无序化学机械转导。

Single molecule-driven nanomotors reveal the dynamic-disordered chemomechanical transduction of active enzymes.

作者信息

Tang Zhuodong, Wu Jingyu, Wu Shaojun, Tang Wenjing, Zhang Jian-Rong, Zhu Wenlei, Zhu Jun-Jie, Chen Zixuan

机构信息

State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, State Key Laboratory of Pollution Control and Resource Reuse, School of Environment, Nanjing University, 163 Xianlin Ave., Nanjing 210023, China.

出版信息

Sci Adv. 2025 Jan 31;11(5):eads0446. doi: 10.1126/sciadv.ads0446.

DOI:10.1126/sciadv.ads0446
PMID:39888997
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11784849/
Abstract

Enzymes facilitate the conversion of chemical energy into mechanical work during biochemical reactions, thereby regulating the dynamic metabolic activity of living systems. However, directly observing the energy release facilitated by fluctuating individual enzymes remains a challenge, leading to a contentious debate regarding the underlying reasons for this phenomenon. Here, we aim to overcome this challenge by developing an oscillating nanomotor powered by a single-molecule enzyme, which allows real-time tracking of energy transduction in enzymatic reactions. Through analysis of the shifts in free energy profiles within the nanomotors, our results unveil not only the heterogeneous energy release patterns of individual enzyme molecules but also the dynamic disorder of a particular enzyme in energy release over extended monitoring periods. By exploring six distinct types of single-molecule enzymatic reactions, we provide the direct evidence supporting the argument that the reaction enthalpy governs the enzymatic energy release. This approach has implications for understanding the mechanism of enzymatic catalysis and developing highly efficient nanomotors.

摘要

酶在生化反应过程中促进化学能向机械功的转化,从而调节生命系统的动态代谢活动。然而,直接观察单个酶波动促进的能量释放仍然是一项挑战,引发了关于这一现象潜在原因的激烈争论。在此,我们旨在通过开发由单分子酶驱动的振荡纳米马达来克服这一挑战,该纳米马达能够实时跟踪酶促反应中的能量转导。通过分析纳米马达内自由能分布的变化,我们的结果不仅揭示了单个酶分子的异质能量释放模式,还揭示了在延长的监测期内特定酶在能量释放方面的动态无序性。通过探索六种不同类型的单分子酶促反应,我们提供了直接证据支持反应焓控制酶促能量释放这一观点。这种方法对于理解酶催化机制和开发高效纳米马达具有重要意义。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5c50/11784849/fadf2e5d9c74/sciadv.ads0446-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5c50/11784849/3e16caa25943/sciadv.ads0446-f1.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5c50/11784849/5bc1a4fbba4d/sciadv.ads0446-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5c50/11784849/fadf2e5d9c74/sciadv.ads0446-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5c50/11784849/3e16caa25943/sciadv.ads0446-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5c50/11784849/e8eebab3f9f7/sciadv.ads0446-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5c50/11784849/910dfea0f026/sciadv.ads0446-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5c50/11784849/5bc1a4fbba4d/sciadv.ads0446-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5c50/11784849/fadf2e5d9c74/sciadv.ads0446-f5.jpg

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Open Questions of Chemically Powered Nano- and Micromotors.化学驱动的纳米和微型马达的开放性问题
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Chemically-powered swimming and diffusion in the microscopic world.微观世界中的化学动力游动与扩散。
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Genetic Perturbation Alters Functional Substates in Alkaline Phosphatase.遗传扰动改变碱性磷酸酶的功能亚基状态。
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