Three different pi-conjugated oligomers (a blue-emitting oligofluorene, a green-emitting oligo(phenylene vinylene), and a red-emitting perylene bisimide) have been functionalized with self-complementary quadruple hydrogen bonding ureidopyrimidinone (UPy) units at both ends. The molecules self-assemble in solution and in the bulk, forming supramolecular polymers. When mixed together in solution, random noncovalent copolymers are formed that contain all three types of chromophores, resulting in energy transfer upon excitation of the oligofluorene energy donor. At a certain mixing ratio, a white emissive supramolecular polymer can be created in solution. In contrast to their unfunctionalized counterparts, bis-UPy-chromophores can easily be deposited as smooth thin films on surfaces by spin coating. No phase separation is observed in these films, and energy transfer is much more efficient than in solution, giving rise to white fluorescence at much lower ratios of energy acceptor to donor. Light emitting diodes based on these supramolecular polymers have been prepared from all three types of pure materials, yielding blue, green, and red devices, respectively. At appropriate mixing ratios of these three compounds, white electroluminescence is observed. This approach yields a toolbox of molecules that can be easily used to construct pi-conjugated supramolecular polymers with a variety of compositions, high solution viscosities, and tuneable emission colors.
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http://dx.doi.org/10.1021/ja807996y | DOI Listing |
Chemistry
January 2025
Indian Institute of Technology Kanpur, Department of Chemistry, Kanpur, 208016, Kanpur, INDIA.
Herein, we report the precise control of molecular to supramolecular chirality induction at the single-molecule level just upon subtle modification in an achiral 'nano-size' trizinc(II) porphyrin trimer. A slight variation in the projection of the substituent at the periphery of the central porphyrin unit in a porphyrin trimer (host) resulted in pronounced changes in the interchromophoric arrangement, leading to distinct 'open' and 'closed' conformations. While 'open' form generates 'monomeric' complex with low CD amplitude, 'closed' form produces exclusive 'polymer' with large, amplified CD signal with opposite sign due to stronger intermolecular excitonic coupling.
View Article and Find Full Text PDFNat Commun
January 2025
Ecole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic Materials, Lausanne, Switzerland.
The plastic waste crisis is among humanity's most urgent challenges. However, widespread adoption of sustainable plastics is hindered by their often inadequate processing characteristics and performance. Here, we introduce a bio-inspired strategy for the modification of a representative high molar mass, biodegradable aliphatic polyester that helps overcome these limitations and remains effective at molar masses far greater than the entanglement molar mass.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Bernal Institute and Department of Chemical Sciences, University of Limerick, Limerick V94 T9PX, Ireland.
2D and 3D porous coordination networks (PCNs) as exemplified by metal-organic frameworks, MOFs, have garnered interest for their potential utility as sorbents for molecular separations and storage. The inherent modularity of PCNs has enabled the development of crystal engineering strategies for systematic fine-tuning of pore size and chemistry in families of related PCNs. The same cannot be said about one-dimensional (1D) coordination polymers, CPs, which are understudied with respect to porosity.
View Article and Find Full Text PDFMater Horiz
January 2025
College of Materials Science and Engineering, State Key Laboratory of Advanced Design and Manufacturing Technology for Vehicle, Hunan University, Changsha, 410082, Hunan, China.
Ionogels are a promising solution to improve the functionality of electrochromic devices (ECDs) by solving issues related to traditional liquid electrolytes, such as volatility, toxicity, and leakage. However, manufacturing ionogels is complicated as it often involves cross-linking polymerization or chemical sol-gel processes, requiring large amounts of inorganic or polymeric gelators. This results in low ionic conductivity and poor ECD performance.
View Article and Find Full Text PDFJ Mater Chem B
January 2025
Department of Cardiology, Sir Run Run Shaw Hospital, Zhejiang University School of Medicine, Hangzhou 310016, China.
Cardiovascular diseases (CVDs) are the foremost cause of mortality worldwide, with incidence and mortality rates persistently climbing despite extensive research efforts. Innovative therapeutic approaches are still needed to extend patients' lives and preserve their health. In the present study, novel supramolecular nanomedicine with both nitric oxide (NO) and antioxidant releasing ability was developed to enhance therapeutic efficacy against vascular injuries.
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