{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,10,1]],"date-time":"2026-10-01T23:23:32Z","timestamp":1790897012931,"version":"4.1.0"},"reference-count":78,"publisher":"American Chemical Society (ACS)","issue":"33","license":[{"start":{"date-parts":[[2026,8,6]],"date-time":"2026-08-06T00:00:00Z","timestamp":1785974400000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"funder":[{"DOI":"10.13039\/501100004281","name":"Narodowe Centrum Nauki","doi-asserted-by":"publisher","award":["2021\/41\/B\/NZ7\/01654"],"award-info":[{"award-number":["2021\/41\/B\/NZ7\/01654"]}],"id":[{"id":"10.13039\/501100004281","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,8,20]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>Solid-state polypeptides undergo continuous conformational reorganization when subjected to various environmental stimuli, reshaping their macroscopic physical behavior. Here, we investigate this phenomenon specifically under thermal treatment using \u03b1-poly-l-lysine hydrobromide (\u03b1-PLL), an ionic polypeptide containing Br\u2013 counterions, as a model system. By combining thermogravimetric analysis (TGA), Fourier-transform infrared (FT-IR) spectroscopy, wide-angle X-ray scattering (WAXS), differential scanning calorimetry (DSC), and broadband dielectric spectroscopy (BDS), we show that freeze-dried \u03b1-PLL initially contains mixed \u03b1-helical, \u03b2-sheet, and \u03b2-turn\/antiparallel \u03b2-sheet conformations. After removal of loosely bound water, thermal treatment drives a transformation toward \u03b2-sheet-rich structures. This process is cooperative and thermally activated, with an apparent activation energy of approximately 64 kJ mol\u20131, indicating that \u03b2-sheet formation requires collective rearrangement of hydrogen-bonded polypeptide chains. The structural transformation is not limited to local changes in secondary structure. WAXS reveals that \u03b1-PLL exhibits liquid-crystalline-like two-dimensional hexagonal packing, which is reorganized in a molecular-weight-dependent manner as \u03b2-sheet-rich architectures develop with increasing temperature. Most importantly, this conformational reorganization produces two unexpected changes in the physical response of \u03b1-PLL. First, the formation of \u03b2-sheet-rich structures is accompanied by a decrease in glass transition temperature (Tg), showing that secondary-structure ordering does not necessarily rigidify the polypeptide matrix. Second, the frequency-dependent conductivity, \u03c3\u2032(f), systematically decreases over a broad frequency range upon annealing, although the \u03b2-sheet-rich state exhibits stronger hydrogen bonds. This suggests that charge transport in \u03b1-PLL is promoted not by the stronger, more static interchain hydrogen-bonding network of \u03b2-sheets, but by the \u03b1-helical state, which may provide a more favorable electrostatic environment for Br\u2013 migration. These findings reveal a direct link between secondary-structure transformation, glass-transition dynamics, mesoscale packing, and ion transport, establishing \u03b1-PLL as a model solid-state polypeptide electrolyte in which conformational reorganization governs both molecular mobility and electrical response.<\/jats:p>","DOI":"10.1021\/acs.jpcb.6c03934","type":"journal-article","created":{"date-parts":[[2026,8,6]],"date-time":"2026-08-06T23:01:27Z","timestamp":1786057287000},"page":"8535-8549","source":"Crossref","is-referenced-by-count":1,"title":["Conformation-Determined\nSegmental Dynamics in \u03b1-Poly-\n                    <scp>l<\/scp>\n                    -Lysine\nHydrobromide: The Impact of Thermally Induced\n\u03b2-Sheet Formation on the Glass Transition Temperature"],"prefix":"10.1021","volume":"130","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-5129-063X","authenticated-orcid":true,"given":"Rafa\u0142","family":"Bielas","sequence":"first","affiliation":[{"name":"Medical University of Silesia in Katowice , , Jagiellon\u0301ska 4 , ,","place":["Sosnowiec, Poland, 41-200"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Anjana","family":"Krishna Sudhakaran Nair Valsala Kumari","sequence":"additional","affiliation":[{"name":"University of Silesia in Katowice , , 75 Pu\u0142ku Piechoty 1 , ,","place":["Chorzo\u0301w, Poland, 41-500"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Krzysztof","family":"Witkowicz","sequence":"additional","affiliation":[{"name":"University of Silesia in Katowice , , Szkolna 9 , ,","place":["Katowice, Poland, 40-006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5888-621X","authenticated-orcid":true,"given":"Anna","family":"Mielan\u0301czyk","sequence":"additional","affiliation":[{"name":"Silesian University of Technology , , B. Krzywoustego 4 , ,","place":["Gliwice, Poland, 44-100"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9444-3114","authenticated-orcid":true,"given":"Magdalena","family":"Tarnacka","sequence":"additional","affiliation":[{"name":"University of Silesia in Katowice , , 75 Pu\u0142ku Piechoty 1 , ,","place":["Chorzo\u0301w, Poland, 41-500"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Anna","family":"Janowska","sequence":"additional","affiliation":[{"name":"University of Silesia in Katowice , , 75 Pu\u0142ku Piechoty 1 , ,","place":["Chorzo\u0301w, Poland, 41-500"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4289-7827","authenticated-orcid":true,"given":"Karolina","family":"Jurkiewicz","sequence":"additional","affiliation":[{"name":"University of Silesia in Katowice , , 75 Pu\u0142ku Piechoty 1 , ,","place":["Chorzo\u0301w, Poland, 41-500"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5871-0203","authenticated-orcid":true,"given":"Kamil","family":"Kamin\u0301ski","sequence":"additional","affiliation":[{"name":"University of Silesia in Katowice , , 75 Pu\u0142ku Piechoty 1 , ,","place":["Chorzo\u0301w, Poland, 41-500"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9886-1076","authenticated-orcid":true,"given":"Barbara","family":"Hachu\u0142a","sequence":"additional","affiliation":[{"name":"University of Silesia in Katowice , , Szkolna 9 , ,","place":["Katowice, Poland, 40-006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9725-8654","authenticated-orcid":true,"given":"Ewa","family":"Kamin\u0301ska","sequence":"additional","affiliation":[{"name":"Medical University of Silesia in Katowice , , Jagiellon\u0301ska 4 , ,","place":["Sosnowiec, Poland, 41-200"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,6]]},"reference":[{"key":"2026082007195838600_cit1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2026.172904","article-title":"Design and Modification Strategies\nfor Peptide-Based Nanomaterials Driven by Antimicrobial Mechanisms","volume":"529","author":"Ding","year":"2026","journal-title":"Chem. 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