RT Journal Article T1 Polyelectrolyte complexes based on a novel and sustainable hemicellulose-rich lignosulphonate for drug delivery applications A1 Dogaris, Ioannis A1 Pylypchuk, Ievgen A1 Henriksson, Gunnar A1 Abbadessa, Anna K1 Polyethylenimine  K1 Chitosan  K1 Lignin  K1 Polyelectrolyte complexation  K1 Controlled drug delivery  K1 Sustainability AB Polyelectrolyte complexes (PECs) are polymeric structures formed by the self-assembly of oppositely charged polymers. Novel biomaterials based on PECs are currently under investigation as drug delivery systems, among other applications. This strategy leverages the ability of PECs to entrap drugs under mild conditions and control their release. In this study, we combined a novel and sustainably produced hemicellulose-rich lignosulphonate polymer (EH, negatively charged) with polyethyleneimine (PEI) or chitosan (CH, positively charged) and agar for the development of drug-releasing PECs. A preliminary screening demonstrated the effect of several parameters (polyelectrolyte ratio, temperature, and type of polycation) on PECs formation. From this, selected formulations were further characterized in terms of thermal properties, surface morphology at the microscale, stability, and ability to load and release methylene blue (MB) as a model drug. EH/PEI complexes had a more pronounced gel-like behaviour compared to the EH/CH complexes. Differential scanning calorimetry (DSC) results supported the establishment of polymeric interactions during complexation. Overall, PECs’ stability was positively affected by low pH, ratios close to 1:1, and the addition of agar. PECs with higher EH content showed a higher MB loading, likely promoted by stronger electrostatic interactions. The EH/CH formulation enriched with agar showed the best sustained release profile of MB during the first 30 h in a pH-dependent environment simulating the gastrointestinal tract. Overall, we defined the conditions to formulate novel PECs based on a sustainable hemicellulose-rich lignosulphonate for potential applications in drug delivery, which promotes the valuable synergy between sustainability and the biomedical field PB Springer SN 2190-393X YR 2024 FD 2024 LK http://hdl.handle.net/10347/33740 UL http://hdl.handle.net/10347/33740 LA eng NO Dogaris, I., Pylypchuk, I., Henriksson, G. et al. Polyelectrolyte complexes based on a novel and sustainable hemicellulose-rich lignosulphonate for drug delivery applications. Drug Deliv. and Transl. Res. (2024). https://doi.org/10.1007/s13346-024-01573-2 NO The authors would like to thank Dr. P. Oinonen and Ecohelix AB for providing samples of the Ecohelix polymer and scientific advice on its use. The research leading to these results was financially supported by Nordforsk, within the Nordic Green Growth Research and Innovation Program (project name: “High-Value Products from Lignin”). A.A. acknowledges funding from ‘la Caixa’ Foundation (ID 100010434) with a fellowship code LCF/BQ/ PR22/11920003. Open Access funding provided thanks to the CRUE-CSIC agreement with Springer Nature. The research leading to these results was financially supported by Nordforsk, within the Nordic Green Growth Research and Innovation Program (project name: “High-Value Products from Lignin”). A.A. acknowledges funding from ‘la Caixa’ Foundation (ID 100010434) with a fellowship code LCF/BQ/ PR22/11920003 DS Minerva RD 24 abr 2026