Department of Chemistry, Key Laboratory of Bioorganic Phosphorus Chemistry & Chemical Biology (Ministry of Education), Tsinghua University, Beijing 100084, China.
Anal Chem. 2022 May 24;94(20):7158-7163. doi: 10.1021/acs.analchem.2c00363. Epub 2022 May 9.
Catalytic enzymes exhibiting enhanced motion have drawn extensive attention over the past decade; nevertheless, little is known about the effect on the environment induced by enzymes. Herein, we studied the active urease system by simultaneously monitoring the diffusion of single anisotropic gold nanorods (AuNRs) with high speed dark-field imaging. We found both the translational and the rotational diffusion coefficients of AuNRs were enhanced but with inconsistent degrees, indicating the catalytic reaction had a minor effect on the physiochemical properties of the environment according to the Stokes-Einstein equation. With the increase of substrate concentration, the diffusion of AuNRs showed increased spatial but decreased temporal heterogeneity. Additionally, high speed imaging revealed AuNRs could experience intermittent ballistic motion for tens of milliseconds. These results imply inhomogeneous distribution of enzymes in free solution induced by active enzymatic reactions.
在过去的十年中,具有增强运动的催化酶引起了广泛关注;然而,对于酶诱导的环境影响知之甚少。在此,我们通过同时监测具有高速暗场成像的单各向异性金纳米棒 (AuNRs) 的扩散来研究活性脲酶体系。我们发现 AuNRs 的平动和转动扩散系数都得到了增强,但增强程度不一致,这表明根据 Stokes-Einstein 方程,催化反应对环境的理化性质影响较小。随着底物浓度的增加,AuNRs 的扩散表现出空间上的增加,但时间上的异质性降低。此外,高速成像显示 AuNRs 可以经历数十毫秒的间歇性弹道运动。这些结果表明,活性酶反应引起的游离溶液中酶的不均匀分布。