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

IF 2.3 2区物理与天体物理 Q3 CHEMISTRY, PHYSICAL Structural Dynamics-Us Pub Date : 2021-09-14 eCollection Date: 2021-09-01 DOI:10.1063/4.0000111

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

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引用次数: 4

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 H₂O and D₂O. 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.

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氧化石墨烯纳米片调控冰形成的结构和动力学机制研究。

最近的研究表明，氧化石墨烯纳米片可以通过控制过冷温度下水中临界冰核的生长来调节冰的形成。此外，氧化石墨烯纳米片作为抗冻蛋白(AFPs)的一个很好的模型系统，其对冰形成机制的研究将有助于揭示抗冻蛋白(AFPs)在自然界中如何调节冰的形成。本文采用时间分辨小角x射线散射(TR-SAXS)和准弹性中子散射(QENS)实验研究氧化石墨烯纳米片调控冰形成的结构和动力学机制。引人注目的是，在TR-SAXS实验中观察到一个瞬态中间态，它只存在于氧化石墨烯尺寸较大(11 nm)的水相分散体中。这证明氧化石墨烯的大小对调节冰的形成至关重要。弹性中子散射结果表明，氧化石墨烯水分散体在H2O和D2O中均存在热滞回现象。QENS提取了氧化石墨烯水分子的结构和动力学信息，揭示了氧化石墨烯水分散体中水分子在接近成冰温度时的不同动力学行为。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Structural Dynamics-Us CHEMISTRY, PHYSICALPHYSICS, ATOMIC, MOLECU-PHYSICS, ATOMIC, MOLECULAR & CHEMICAL

CiteScore

5.50

自引率

3.60%

发文量

审稿时长

16 weeks

期刊介绍： Structural Dynamics focuses on the recent developments in experimental and theoretical methods and techniques that allow a visualization of the electronic and geometric structural changes in real time of chemical, biological, and condensed-matter systems. The community of scientists and engineers working on structural dynamics in such diverse systems often use similar instrumentation and methods. The journal welcomes articles dealing with fundamental problems of electronic and structural dynamics that are tackled by new methods, such as: Time-resolved X-ray and electron diffraction and scattering, Coherent diffractive imaging, Time-resolved X-ray spectroscopies (absorption, emission, resonant inelastic scattering, etc.), Time-resolved electron energy loss spectroscopy (EELS) and electron microscopy, Time-resolved photoelectron spectroscopies (UPS, XPS, ARPES, etc.), Multidimensional spectroscopies in the infrared, the visible and the ultraviolet, Nonlinear spectroscopies in the VUV, the soft and the hard X-ray domains, Theory and computational methods and algorithms for the analysis and description of structuraldynamics and their associated experimental signals. These new methods are enabled by new instrumentation, such as: X-ray free electron lasers, which provide flux, coherence, and time resolution, New sources of ultrashort electron pulses, New sources of ultrashort vacuum ultraviolet (VUV) to hard X-ray pulses, such as high-harmonic generation (HHG) sources or plasma-based sources, New sources of ultrashort infrared and terahertz (THz) radiation, New detectors for X-rays and electrons, New sample handling and delivery schemes, New computational capabilities.