Imaging a solvent-swollen polymer gel network by open liquid transmission electron microscopy

Srivastava, Satyam; Ribbe, Alexander E.; Russell, Thomas P.; Hoagland, David A.

doi:10.1002/pol.20230907

Title: Imaging a solvent-swollen polymer gel network by open liquid transmission electron microscopy

Journal Article · 18 March 2024 · Journal of Polymer Science

DOI: https://doi.org/10.1002/pol.20230907 · OSTI ID:2429600

^[1]; Ribbe, Alexander E. ^[1];

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Univ. of Massachusetts, Amherst, MA (United States)
Univ. of Massachusetts, Amherst, MA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Tohoku Univ., Sendai (Japan)

Visualizing the network of a solvent-swollen polymer gel remains problematic. To address this challenge, open transmission electron microscopy (TEM) was applied to thin gel films permeated by a nonvolatile ionic liquid. The targeted physical gels were prepared by cooling concentrated solutions of poly(ethylene glycol) in 1-ethyl-3-methyl imidazolium ethyl sulfate [EMIM][EtSO₄]. During the cooling, gelation occurred by a frustrated crystallization of the dissolved polymer, leading to a percolated, solvent-permeated semicrystalline network in which nanoscale polymer crystals acted as crosslinks. Crystalline features ranging from ~5 to ~200 nm were observed, with the visible network strands dominantly consisting of long curvilinear crystallites of ~15–20 nm diameter. Nascent spherulites irregularly decorated the network, creating a complex structural hierarchy that complicated analyses. Lacking diffraction contrast, TEM did not visualize the many disordered, fully solvated PEG chains present in the voids between crystals. Finally, recognizing that a network's three dimensionality is ambiguous when assessed through two-dimensional microscopy projections, a small gel region was studied by TEM tomography, revealing a nearly isotropic three-dimensional arrangement of the curvilinear crystallites, which displayed remarkably uniform cylindrical cross sections.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 2429600

Journal Information:: Journal of Polymer Science, Journal Name: Journal of Polymer Science Journal Issue: 16 Vol. 62; ISSN 2642-4150

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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