PMID- 36846500 OWN - NLM STAT- PubMed-not-MEDLINE LR - 20230228 IS - 0883-7694 (Print) IS - 1938-1425 (Electronic) IS - 0883-7694 (Linking) VI - 47 IP - 12 DP - 2022 TI - Ionic poly(dimethylsiloxane)-silica nanocomposites: Dispersion and self-healing. PG - 1185-1197 LID - 10.1557/s43577-022-00346-x [doi] AB - ABSTRACT: Poly(dimethylsiloxane) (PDMS)-based nanocomposites have attracted increasing attention due to their inherent outstanding properties. Nevertheless, the realization of high levels of dispersion of nanosilicas in PDMS represents a challenge arising from the poor compatibility between the two components. Herein, we explore the use of ionic interactions located at the interface between silica and a PDMS matrix by combining anionic sulfonate-functionalized silica and cationic ammonium-functionalized PDMS. A library of ionic PDMS nanocomposites was synthesized and characterized to highlight the impact of charge location, density, and molecular weight of ionic PDMS polymers on the dispersion of nanosilicas and the resulting mechanical reinforcement. The use of reversible ionic interactions at the interface of nanoparticles-polymer matrix enables the healing of scratches applied to the surface of the nanocomposites. Molecular dynamics simulations were used to estimate the survival probability of ionic cross-links between nanoparticles and the polymer matrix, revealing a dependence on polymer charge density. IMPACT STATEMENT: Poly(dimethylsiloxane) (PDMS) has been widely used in diverse applications due to its inherent attractive and multifunctional properties including optical transparency, high flexibility, and biocompatibility. The combination of such properties in a single polymer matrix has paved the way toward a wide range of applications in sensors, electronics, and biomedical devices. As a liquid at room temperature, the cross-linking of the PDMS turns the system into a mechanically stable elastomer for several applications. Nanofillers have served as a reinforcing agent to design PDMS nanocomposites. However, due to significant incompatibility between silica and the PDMS matrix, the dispersion of nanosilica fillers has been challenging. One of the existing strategies to improve nanoparticle dispersion consists of grafting oppositely charged ionic functional groups to the nanoparticle surface and the polymer matrix, respectively, creating nanoparticle ionic materials. Here, this approach has been explored further to improve the dispersion of nanosilicas in a PDMS matrix. The designed ionic PDMS nanocomposites exhibit self-healing properties due to the reversible nature of ionic interactions. The developed synthetic approach can be transferred to other kinds of inorganic nanoparticles dispersed in a PDMS matrix, where dispersion at the nanometer scale is a prerequisite for specific applications such as encapsulants for light-emitting diodes (LEDs). SUPPLEMENTARY INFORMATION: The online version contains supplementary material available at 10.1557/s43577-022-00346-x. CI - (c) The Author(s) 2022. FAU - Mugemana, Clement AU - Mugemana C AD - Materials Research and Technology, Luxembourg Institute of Science and Technology, Esch-sur-Alzette, Luxembourg. GRID: grid.423669.c FAU - Moghimikheirabadi, Ahmad AU - Moghimikheirabadi A AD - Polymer Physics, Department of Materials, ETH Zurich, Zurich, Switzerland. GRID: grid.5801.c. ISNI: 0000 0001 2156 2780 FAU - Arl, Didier AU - Arl D AD - Materials Research and Technology, Luxembourg Institute of Science and Technology, Esch-sur-Alzette, Luxembourg. GRID: grid.423669.c FAU - Addiego, Frederic AU - Addiego F AD - Materials Research and Technology, Luxembourg Institute of Science and Technology, Esch-sur-Alzette, Luxembourg. GRID: grid.423669.c FAU - Schmidt, Daniel F AU - Schmidt DF AD - Materials Research and Technology, Luxembourg Institute of Science and Technology, Esch-sur-Alzette, Luxembourg. GRID: grid.423669.c FAU - Kroger, Martin AU - Kroger M AD - Polymer Physics, Department of Materials, ETH Zurich, Zurich, Switzerland. GRID: grid.5801.c. ISNI: 0000 0001 2156 2780 FAU - Karatrantos, Argyrios V AU - Karatrantos AV AUID- ORCID: 0000-0002-3169-6894 AD - Materials Research and Technology, Luxembourg Institute of Science and Technology, Esch-sur-Alzette, Luxembourg. GRID: grid.423669.c LA - eng PT - Journal Article DEP - 20220916 PL - England TA - MRS Bull JT - MRS bulletin JID - 100971398 PMC - PMC9947054 OTO - NOTNLM OT - Composite OT - Inorganic and simulation OT - Interface OT - Nanoscale COIS- Conflict of interestThe authors declare that there is no conflict of interest. EDAT- 2023/02/28 06:00 MHDA- 2023/02/28 06:01 PMCR- 2022/09/16 CRDT- 2023/02/27 05:55 PHST- 2022/05/13 00:00 [accepted] PHST- 2023/02/27 05:55 [entrez] PHST- 2023/02/28 06:00 [pubmed] PHST- 2023/02/28 06:01 [medline] PHST- 2022/09/16 00:00 [pmc-release] AID - 346 [pii] AID - 10.1557/s43577-022-00346-x [doi] PST - ppublish SO - MRS Bull. 2022;47(12):1185-1197. doi: 10.1557/s43577-022-00346-x. Epub 2022 Sep 16.