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通过电子自旋共振(ESR)和正电子湮没寿命谱(PALS)研究正丙醇在规整MCM-41基质中受限的分子探针动力学和自由体积不均匀性。

Molecular probe dynamics and free volume heterogeneities in n-propanol confined in a regular MCM-41 matrix by ESR and PALS.

作者信息

Bartoš Josef, Švajdlenková Helena, Šauša Ondrej

机构信息

Polymer Institute of SAS Dúbravská Cesta 9 SK-845 41 Bratislava Slovakia

Institute of Physics of SAS Dúbravská Cesta 9 SK-845 11 Bratislava Slovakia.

出版信息

RSC Adv. 2020 Jan 13;10(4):2283-2294. doi: 10.1039/c9ra09495d. eCollection 2020 Jan 8.

DOI:10.1039/c9ra09495d
PMID:35494603
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9048748/
Abstract

A combined investigation of the spin probe TEMPO mobility and the free volume holes in -propanol (-PrOH) confined in a regular virgin MCM-41 matrix by means of ESR or PALS techniques, respectively, is reported. Dynamics of spin probe TEMPO alters at several characteristic ESR temperatures which are close to the characteristic PALS ones reflecting the changes in -Ps annihilation and the related free volume. Correlations between these characteristic ESR and PALS temperatures indicate the common physical origins of the respective changes in the free volume expansion and the TEMPO mobility in the confined liquid -PrOH. The significant difference in dynamic heterogeneity of TEMPO after confinement and free volume dispersion reflect the strongly altered structural-dynamic relationships in the confined -PrOH medium with respect to the bulk situation.

摘要

本文报道了分别通过电子自旋共振(ESR)或正电子湮没寿命谱(PALS)技术,对限制在规整原始MCM-41基质中的异丙醇(-PrOH)中自旋探针TEMPO的迁移率和自由体积空穴进行的联合研究。自旋探针TEMPO的动力学在几个特征ESR温度下发生变化,这些温度与特征PALS温度相近,反映了正电子素(-Ps)湮没的变化及相关自由体积的变化。这些特征ESR和PALS温度之间的相关性表明,受限液体-PrOH中自由体积膨胀和TEMPO迁移率各自变化具有共同的物理起源。受限后TEMPO动态不均匀性和自由体积分散的显著差异反映出,相对于本体情况,受限-PrOH介质中结构-动力学关系发生了强烈改变。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c396/9048748/0d8b81bf9396/c9ra09495d-f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c396/9048748/aba8e934acc9/c9ra09495d-f1.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c396/9048748/b656bce80501/c9ra09495d-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c396/9048748/065283f40781/c9ra09495d-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c396/9048748/777bca97eae9/c9ra09495d-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c396/9048748/38166bc30f78/c9ra09495d-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c396/9048748/0d8b81bf9396/c9ra09495d-f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c396/9048748/aba8e934acc9/c9ra09495d-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c396/9048748/b54313ee8b36/c9ra09495d-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c396/9048748/b656bce80501/c9ra09495d-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c396/9048748/065283f40781/c9ra09495d-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c396/9048748/777bca97eae9/c9ra09495d-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c396/9048748/38166bc30f78/c9ra09495d-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c396/9048748/0d8b81bf9396/c9ra09495d-f7.jpg

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Phys Chem Chem Phys. 2017 Jun 14;19(23):15215-15226. doi: 10.1039/c7cp00446j.
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