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Water Dynamics in NH2-MIL-125: Insights from a Combined 1H NMR Relaxometry and Computational Investigation
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2021-06-25 , DOI: 10.1021/acs.jpcc.1c02045
Silvia Pizzanelli 1 , Angelo Freni 1 , Amir H. Farmahini 2 , Larisa G. Gordeeva 3, 4 , Lev Sarkisov 2 , Marina V. Solovyeva 3 , Claudia Forte 1
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2021-06-25 , DOI: 10.1021/acs.jpcc.1c02045
Silvia Pizzanelli 1 , Angelo Freni 1 , Amir H. Farmahini 2 , Larisa G. Gordeeva 3, 4 , Lev Sarkisov 2 , Marina V. Solovyeva 3 , Claudia Forte 1
Affiliation
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The dynamics of water confined in a microporous metal–organic framework was investigated by 1H fast field-cycling nuclear magnetic resonance (NMR) relaxometry, exploring time scales ranging between 10 μs and 0.1 ns in the 25–80 °C temperature interval. The data were interpreted within a dynamic model where molecules bind to the surface hopping among preferential binding sites. The bound molecules are also subject to local faster reorientations. Numerical analysis of the data allowed the characteristic times associated with hops and local anisotropic reorientations to be determined together with their activation energies, as derived through Arrhenius fits. The values of the activation energies, 16 ± 2 and 4.5 ± 0.5 kJ/mol, respectively, were rationalized within the model. 1H magic-angle spinning NMR was used to quantify the water loading level and to obtain evidence on the presence of bound water molecules as required by the dynamic model, whereas molecular simulations were conducted to obtain complementary information on relevant properties, such as the porosity of the matrix, the water binding sites, self-diffusion, and interaction energies in the confined space.
中文翻译：
NH 2 -MIL-125 中的水动力学：结合1 H NMR 弛豫测量和计算研究的见解
通过1 H 快速场循环核磁共振 (NMR) 弛豫测量法研究了限制在微孔金属-有机框架中的水的动力学，探索了 25-80°C 温度区间内 10 μs 和 0.1 ns 之间的时间尺度。在动态模型中解释数据，其中分子结合到优先结合位点之间的表面跳跃。结合的分子也受到局部更快的重新定向。数据的数值分析允许确定与跳跃和局部各向异性重定向相关的特征时间及其激活能，如通过 Arrhenius 拟合得出的。活化能的值分别为 16 ± 2 和 4.5 ± 0.5 kJ/mol，在模型内进行了合理化。1H 魔角旋转 NMR 用于量化水负载水平，并根据动态模型的要求获得关于结合水分子存在的证据，而进行分子模拟以获得相关特性的补充信息，例如孔隙率基质、水结合位点、自扩散和密闭空间中的相互作用能。
更新日期：2021-07-08
中文翻译：
NH 2 -MIL-125 中的水动力学：结合1 H NMR 弛豫测量和计算研究的见解
通过1 H 快速场循环核磁共振 (NMR) 弛豫测量法研究了限制在微孔金属-有机框架中的水的动力学，探索了 25-80°C 温度区间内 10 μs 和 0.1 ns 之间的时间尺度。在动态模型中解释数据，其中分子结合到优先结合位点之间的表面跳跃。结合的分子也受到局部更快的重新定向。数据的数值分析允许确定与跳跃和局部各向异性重定向相关的特征时间及其激活能，如通过 Arrhenius 拟合得出的。活化能的值分别为 16 ± 2 和 4.5 ± 0.5 kJ/mol，在模型内进行了合理化。1H 魔角旋转 NMR 用于量化水负载水平，并根据动态模型的要求获得关于结合水分子存在的证据，而进行分子模拟以获得相关特性的补充信息，例如孔隙率基质、水结合位点、自扩散和密闭空间中的相互作用能。
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