Host-guest interactions and confinement effects in HZSM-5 and chabazite zeolites studied by low-field NMR spin relaxation

Host-guest interactions and confinement effects in HZSM-5 and chabazite zeolites studied by low-field NMR spin relaxation
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通过低场核磁共振自旋弛豫研究 HZSM-5 和菱沸石中的主客体相互作用和限制效应

DOI:
10.1016/j.mtchem.2022.100901
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发表时间:
2022
影响因子:
7.3
通讯作者:
D'Agostino C
D'Agostino C
中科院分区:
化学2区
文献类型:
--
作者:
D'Agostino C

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多孔材料中流体/固体相互作用的表征对于其设计和优化至关重要,特别是在吸附和催化等应用中。然而,探测受限于多孔系统中的流体的界面现象特别具有挑战性。核磁共振(NMR)自旋弛豫是近年来出现的一种快速、非侵入性的实验技术,用于探测介孔催化材料中吸附质/吸附剂的相互作用。最近,在高场(300 MHz)超导磁体上进行的NMR弛豫测量已被成功地验证为表征HZSM-5沸石中酸性的稳健方法。在低场、台式NMR仪器的背景下扩展这样的技术将是非常有益的,因为它将使NMR弛豫成为用于沸石和微孔材料中的吸附物/吸附剂相互作用的非侵入性、快速表征的更有吸引力和更容易获得的工具。在此,我们验证了使用低场,台式NMR自旋弛豫作为表征微孔沸石材料中的主客体相互作用的指标,使用水作为限制在两种不同的沸石框架,HZSM-5和菱沸石,具有不同的二氧化硅/氧化铝比的客体分子。这里报道的结果表明,低场NMR弛豫测量作为表征微孔材料中吸附和分子动力学的快速筛选工具的鲁棒性和灵敏度,对学术界和工业界都具有重要意义,使该方法更广泛地使用,从而扩大了材料化学和表征的工具集。
The characterization of fluid/solid interactions in porous materials is crucial for their design and optimization, most notably in applications such as adsorption and catalysis. Yet, probing interfacial phenomena of fluids confined in porous systems is particularly challenging. Nuclear magnetic resonance (NMR) spin relaxation has emerged in recent years as a rapid, non-invasive experimental technique to probe adsorbate/adsorbent interactions in mesoporous catalytic materials. More recently, NMR relaxation measurements performed on high-field (300 MHz) superconducting magnets have been successfully validated as a robust method to characterize acidity in HZSM-5 zeolites. Expanding such techniques in the context of low-field, bench-top NMR instruments would be highly beneficial as it would make NMR relaxation a much more appealing and accessible tool for non-invasive, rapid characterization of adsorbate/adsorbent interactions in zeolites and microporous materials. Herein, we validate the use of low-field, bench-top NMR spin relaxation as an indicator for characterizing host-guest interactions in microporous zeolitic materials, using water as guest molecules confined within two different zeolite frameworks, HZSM-5 and chabazite, with varying silica/alumina ratio. The results reported here demonstrate the robustness and sensitivity of low-field NMR relaxation measurements as a rapid screening tool for characterizing adsorption and molecular dynamics in microporous materials, with important implications for both academics and industrialists in terms of making the method more widely accessible, hence expanding the set of tools for materials chemistry and characterization.
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