Faraone Antonio, Liu Kao-Hsiang, Mou Chung-Yuan, Zhang Yang, Chen Sow-Hsin
NIST Center for Neutron Research, National Institute for Standards and Technology, Gaithersburg, Maryland 20899-6102, USA.
J Chem Phys. 2009 Apr 7;130(13):134512. doi: 10.1063/1.3097800.
The single particle dynamics of water confined in a hydrophobically modified MCM-41-S sample has been studied using three high resolution quasielastic neutron scattering spectrometers in the temperature range from 300 to 210 K. A careful modeling of the dynamics allowed us to obtain good agreement among the results obtained with the three instruments, which have very different energy resolutions. The picture arising from the data is that, because of the heterogenous environment experienced by the water molecules, the dynamics show a broad distribution of relaxation times. However, the Fickian diffusive behavior is retained. In the investigated temperature range we found no evidence of the dynamic crossover, from a non-Arrhenius to an Arrhenius behavior, which was detected for water confined in hydrophilic MCM-41-S. This finding is in agreement with what was reported by Chu et al. [Phys. Rev. E 76, 021505 (2007)] for water confined in other hydrophobic confining media that the dynamic crossover takes place at a much lower temperature. The results reported in the paper help clarify the role that the chemical interaction between the water molecules and the walls of the confining host plays in determining the characteristics of the water dynamics, as compared to purely geometric constraints such as the size and shape of the pores.
利用三台高分辨率准弹性中子散射光谱仪,在300至210 K的温度范围内,研究了疏水改性MCM - 41 - S样品中受限水的单粒子动力学。通过对动力学进行细致建模,我们得以在三台能量分辨率差异很大的仪器所获得的结果之间取得良好的一致性。数据呈现出的情况是,由于水分子所处环境的不均匀性,动力学表现出弛豫时间的广泛分布。然而,菲克扩散行为得以保留。在研究的温度范围内,我们没有发现动态转变的证据,即从非阿仑尼乌斯行为转变为阿仑尼乌斯行为,而在亲水MCM - 41 - S中受限的水则检测到了这种转变。这一发现与Chu等人[《物理评论E》76, 021505 (2007)]所报道的结果一致,即在其他疏水受限介质中受限的水,动态转变发生在低得多的温度下。本文所报道的结果有助于阐明水分子与受限主体壁之间的化学相互作用,相较于诸如孔隙大小和形状等纯粹的几何约束,在决定水动力学特性方面所起的作用。