957 lines
81 KiB
Text
957 lines
81 KiB
Text
<!DOCTYPE html>
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<h1 class="nist-page__title">Assessing Composite Structure in Metal-Organic Framework-Polymer Mixed-Matrix Membranes</h1>
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<div class="nist-field__label">Published</div>
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<div class="nist-field__item"><time datetime="2024-03-15T12:00:00Z">March 15, 2024</time>
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<div class="nist-field__item"><span class="nist-author">Avery Baumann</span>, <span class="nist-author">Peter Beaucage</span>, Richard Vallery, David Gidley, <span class="nist-author">Ryan Nieuwendaal</span>, <span class="nist-author">Chad R. Snyder</span>, Jan Ilavsky, Fu Chen, <span class="nist-author">Christopher Stafford</span>, <span class="nist-author">Christopher Soles</span></div>
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<h3>Abstract</h3>
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Metal-organic frameworks (MOFs) are renowned for their tunable structure, porosity, and internal chemistry with demonstrated applications in molecular separations, storage, and conversion. While they are widely usable, the powdery characteristics of MOF materials can be limiting for large-scale processing and implementation in devices. Incorporating MOF particles into polymer supports affords engineering solutions to overcome these issues, yet the nature of the resulting composites is difficult to assess. In this work, we present spectroscopic and calorimetric methods that we believe help establish a holistic physicochemical picture of the composite structure using a series of Zr MOFs with different pore sizes as a testbed. Power law decays are observed in X-ray scattering profiles in low q-space ranging between 2.4 to 3.3, which we interpret as changes in scattering due to polymer infiltrating MOF particles. This interpretation is supported by solid-state nuclear magnetic resonance spectroscopy and differential scanning calorimetry measurements that identify populations of MOF-associated polymer. Additionally, positron annihilation lifetime spectroscopy measurements collected on a series of composites with different MOF-polymer ratios show multiple decay constants each correlated to a different free volume element. In combination with the spectroscopic, calorimetric and scattering results, we utilize the trends in decay constants as a function of polymer mass fraction to hypothesize a polymer infiltration mechanism whereby large pores are preferentially filled, followed by small pores and, later still, interstitial spaces between particles. Even with vigorous investigation of polymer, MOF, and interface characteristics, the complex and heterogeneous nature of the composites makes absolute structural assertions difficult. We envision the approaches demonstrated here will be a useful foundation to assess and ultimately guide the design of future MOF-polymer composites.
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<div class="nist-field__item">Chemistry of Materials</div>
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<div class="nist-field__item"><a href="https://doi.org/10.1021/acs.chemmater.4c00283" target="_blank">https://doi.org/10.1021/acs.chemmater.4c00283</a></div>
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<h3 class="nist-field__label">Keywords</h3>
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<div class="nist-field__item">Metal-organic framework, polymer, composite, X-ray scattering, spectroscopy</div>
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Baumann, A.
|
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, Beaucage, P.
|
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, Vallery, R.
|
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, Gidley, D.
|
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, Nieuwendaal, R.
|
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, Snyder, C.
|
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, Ilavsky, J.
|
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, Chen, F.
|
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, Stafford, C.
|
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and Soles, C.
|
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|
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(2024),
|
||
Assessing Composite Structure in Metal-Organic Framework-Polymer Mixed-Matrix Membranes, Chemistry of Materials, [online], https://doi.org/10.1021/acs.chemmater.4c00283, https://tsapps.nist.gov/publication/get_pdf.cfm?pub_id=936777
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(Accessed March 4, 2025)
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Created March 15, 2024
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