Functional Group Resolved Nuclear Spin Relaxation in Porous Media

02 July 2021, Version 2
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

Understanding solid-fluid interactions within porous materials is critical for their efficient utilisation across chemical reaction and separation processes. However, detailed characterisation of interfacial phenomena within such systems is hampered by their optically opaque nature. Motivated by the need to bridge this capability gap, we detail here the application of low magnetic field 2D 1H nuclear spin relaxation measurements as a non-invasive probe of sorbate/sorbent interactions, exploring the relaxation characteristics exhibited by liquid adsorbates confined to a model mesoporous silica. For the first time, we demonstrate the capacity of such measurements to distinguish functional group-specific relaxation phenomena across a diverse range of protic adsorbates of wide importance as solvents, reagents, and hydrogen carriers, with distinct relaxation environments assigned to the alkyl and hydroxyl moieties of the confined liquids. Uniquely, this relaxation behaviour is shown to correlate with adsorbate acidity, with the observed relationship rationalised on the basis of surface-adsorbate proton exchange dynamics.

Keywords

NMR relaxation
porous materials
adsorption

Supplementary materials

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Preprint Supplementary Information
Description
Supplementary discussion containing: • Supplementary Note 1: Surface Relaxation Theory • Supplementary Note 2: Methanol-d4 Exchange Experiments • Supplementary Table 1 • Supplementary Figures 1 – 3
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