Poly-3-hydroxybutyrate, a crystal-mobile biodegradable polyester

<p>This Dataset comprises&nbsp;the raw data contained in the figures of our journal article in&nbsp;<em>Macromolecules </em>(DOI: 10.1021/acs.macromol.4c00938) and its Supporting Information (SI)<em>.&nbsp;</em>We provide a preprint of the initially submitted article including the SI for reference to the figures and their captions, necessary to use the data. Note that a few figures have changed upon revision, so please also check the published article. For copyright details and licensing we refer to the published article and the publisher. Here is the abstract of the article:</p> <p>Poly(3-hydroxybutyrate), a biodegradable thermoplastic with potential to partially replace oil-based commodities, suffers from embrittlement over storage time. We here investigate possible causes by monitoring changes in mechanical and thermal properties as well as the semicrystalline morphology (crystallinity, lamellar stack dimensions and its inhomogeneity) over time, using advanced small-angle X-ray scattering analyses for the latter. We find that the slow rise in the shear modulus of the materials is accompanied by secondary crystallization, detected as a lamellar thickening and an increase of the melting point. These morphology changes may be due to chain mobility in the crystallites. This is a feature of "crystal-mobile" polymers that are known to be able to crystallize more fully than their crystal-fixed counterparts. We present first evidence of the related crystalline <em>&alpha;_c</em>-relaxation in P3HB by dynamic-mechanical analysis (DMA) and investigate the process microscopically by advanced magic-angle spinning solid-state exchange NMR techniques, specifically centerband-only detection of exchange. We show that monomer jumps in the P3HB crystals are comparably slow (i.e., with an average correlation time&nbsp;<em>&tau;_c</em>&nbsp; of 0.1 s at 120 &deg;C). Their apparent activation energy (80-90 kJ/mol) is found to be independent of the crystallization temperature and in good agreement with the DMA results.</p>