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氧化石墨烯纳米片调控冰形成的结构与动力学机制研究

Investigations of structural and dynamical mechanisms of ice formation regulated by graphene oxide nanosheets.

作者信息

Zhang Shengkai, Han Jingjing, Luo Xiang, Wang Zhixin, Gu Xudong, Li Na, de Souza Nicolas R, Garcia Sakai Victoria, Chu Xiang-Qiang

机构信息

Graduate School of China Academy of Engineering Physics, Beijing, China.

National Facility for Protein Science in Shanghai, Zhangjiang Laboratory, Shanghai Advanced Research Institute, CAS, No.333, Haike Road, Shanghai 201210, China.

出版信息

Struct Dyn. 2021 Sep 14;8(5):054901. doi: 10.1063/4.0000111. eCollection 2021 Sep.

Abstract

Recent research indicates that graphene oxide (GO) nanosheets can be used to regulate ice formation by controlling critical ice nucleus growth in water at supercooling temperatures. In addition, the study of ice formation mechanisms regulated by GO nanosheets, a good model system for antifreeze proteins (AFPs), will shed light on how AFPs regulate ice formation in nature. In this work, time-resolved small-angle x-ray scattering (TR-SAXS) and quasi-elastic neutron scattering (QENS) experiments were carried out to investigate the structural and dynamical mechanisms of ice formation regulated by GO nanosheets. Strikingly, a transient intermediate state was observed in TR-SAXS experiments that only exists in the aqueous dispersions with a larger GO size (11 nm). This serves as evidence that the size of GO is critical for regulating ice formation. Elastic neutron scattering results indicate that ice is formed in all samples and thermal hysteresis occurs in GO aqueous dispersions in both HO and DO. The structural and dynamics information about water molecules in GO, extracted from QENS, reveals different dynamical behaviors of water molecules in GO aqueous dispersions when approaching the ice formation temperature.

摘要

近期研究表明,氧化石墨烯(GO)纳米片可通过控制过冷温度下水体中临界冰核的生长来调控冰的形成。此外,对由GO纳米片调控的冰形成机制的研究,作为抗冻蛋白(AFP)的一个良好模型系统,将有助于揭示AFP在自然界中如何调控冰的形成。在这项工作中,进行了时间分辨小角X射线散射(TR-SAXS)和准弹性中子散射(QENS)实验,以研究由GO纳米片调控的冰形成的结构和动力学机制。令人惊讶的是,在TR-SAXS实验中观察到一个瞬态中间态,该状态仅存在于具有较大GO尺寸(11纳米)的水分散体中。这证明了GO的尺寸对于调控冰的形成至关重要。弹性中子散射结果表明,所有样品中都形成了冰,并且在H₂O和D₂O的GO水分散体中都出现了热滞现象。从QENS中提取的关于GO中水分子的结构和动力学信息,揭示了在接近冰形成温度时,GO水分散体中水分子的不同动力学行为。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8588/8443304/a0ae9a2f1b49/SDTYAE-000008-054901_1-g001.jpg

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