The features of well-conjugated and planar aromatic structures make π-conjugated luminescent materials suffer from aggregation caused quenching (ACQ) effect when used in solid or aggregated states, which greatly impedes their applications in optoelectronic devices and biological applications. Herein, we reduce the ACQ effect by demonstrating a facile and low cost method to co-assemble polycyclic aromatic hydrocarbon (PAH) chromophores and octafluoronaphthalene together. Significantly, the solid photoluminescence quantum yield (PLQYs) for the as-resulted four micro/nanococrystals are enhanced by 254%, 235%, 474 and 582%, respectively. Protection from hydrophilic polymer chains (P123 (PEO20-PPO70-PEO20)) endows the cocrystals with superb dispersibility in water. More importantly, profiting from the above-mentioned highly improved properties, nano-cocrystals present good biocompatibility and considerable cell imaging performance. This research provides a simple method to enhance the emission, biocompatibility and cellular permeability of common chromophores, which may open more avenues for the applications of originally non- or poor fluorescent PAHs.
Organic thermoelectric (TE) materials can directly convert heat to electricity, and they are emerging as new materials for energy harvesting and cooling technologies. The performance of TE materials mainly depends on the properties of materials, including the Seebeck coefficient, electrical conductivity, thermal conductivity, and thermal stability. Traditional TE materials are mostly based on low-bandgap inorganic compounds, such as bismuth chalcogenide, lead telluride, and tin selenide, while organic materials as promising TE materials are attracting more and more attention because of their intrinsic advantages, including cost-effectiveness, easy processing, low density, low thermal conductivity, and high flexibility. However, to meet the requirements of practical applications, the performance of organic TE materials needs much improvement. A variety of efforts have been made to enhance the performance of organic TE materials, including the modification of molecular structure, and chemical or electrochemical doping. In this review, we summarize recent progress in organic TE materials, and discuss the feasible strategies for enhancing the properties of organic TE materials for future energy-harvesting applications.
Searching new organic cathode materials to address the issues of poor cycle stability and low capacity in lithium ion batteries (LIBs) is very important and highly desirable. In this research, a 2D boroxine‐linked chemically‐active pyrene‐4,5,9,10‐tetraone (PTO) covalent organic framework (2D PPTODB COFs) was synthesized as an organic cathode material with remarkable electrochemical properties, including high electrochemical activity (four redox electrons), safe oxidation potential window (between 2.3 and 3.08 V vs. Li/Li+), superb structural/chemical stability, and strong adhesiveness. A binder‐free cathode was obtained by mixing 70 wt % PPTODB and 30 wt % carbon nanotubes (CNTs) as a conductive additive. Promoted by the fast kinetics of electrons/ions, high electrochemical activity, and effective π–π interaction between PPTODB and CNTs, LIBs with the as‐prepared cathode exhibited excellent electrochemical performance: a high specific capacity of 198 mAh g−1, a superb rate ability (the capacity at 1000 mA g−1 can reach 76 % of the corresponding value at 100 mA g−1), and a stable coulombic efficiency (≈99.6 % at the 150th cycle). This work suggests that the concept of binder‐free 2D electroactive materials could be a promising strategy to approach energy storage with high energy density.
Lithium-ion batteries (LIBs) have been demonstrated as one of the most promising energy storage devices for applications in electric vehicles, smart grids, large-scale energy storage systems, and portable electronics.
Two ruthenium atoms are covalently connected to the para positions of a phenyl ring in 1,2,4,5-tetra(2-pyridyl)benzene (tpb) to form a linear Ru-tpb-Ru arrangement. This unique structure leads to appealing electronic properties for the biscyclometalated complex [(tpy)Ru(tpb)Ru(tpy)](2+), where tpy is 2,2';6',2″-terpyridine. It could be stepwise oxidized at substantially low potential (+0.12 and +0.55 V vs Ag/AgCl) and with a noticeably large comproportionation constant (1.94 × 10(7)). In addition to the routinely observed metal-to-ligand charge-transfer transitions, [(tpy)Ru(tpb)Ru(tpy)](2+) displays a separate and distinct absorption band at 805 nm with appreciable absorptivity (ε = 9000 M(-1) cm(-1)). This band is assigned to the charge transition from the Ru-tpb-Ru motif to the pyridine rings of tpb with the aide of density functional theory (DFT) and time-dependent DFT calculations. Complex [(tpy)Ru(tpb)Ru(tpy)](2+) was precisely titrated with 1 equiv of cerium ammonium nitrate to produce [(tpy)Ru(tpb)Ru(tpy)](3+), which shows intense multiple NIR transitions. The electronic coupling parameters H(ab) of individual NIR components are determined to be 5812, 4942, 4358, and 3560 cm(-1). DFT and TDDFT calculation were performed on [(tpy)Ru(tpb)Ru(tpy)](3+) to elucidate its electronic structure and spin density population and the nature of the observed NIR transitions. Electron paramagnetic resonance studies of [(tpy)Ru(tpb)Ru(tpy)](3+) exhibit a discernible rhombic signal with the isotropic g factor of ⟨g⟩ = 2.144. These results point to the strong orbital interaction of tpb with metal centers and that tpb behaves as a redox noninnocent bridging ligand in [(tpy)Ru(tpb)Ru(tpy)](2+). Complex [(tpy)Ru(tpb)Ru(tpy)](3+) is determined to be a Robin-Day class III system with full charge delocalization across the Ru-tpb-Ru motif.
A 1,4-benzene-bridged covalent hybrid of triarylamine and cyclometalated ruthenium 1(2+) was isolated as a bench-stable open-shell substance. The free spin in this complex is mainly associated with the triarylamine unit, as indicated by EPR and DFT calculations and electrochemical analysis. It exhibits an intense intervalence-charge-transfer transition around 1050 nm that is not present in 1(+) and 1(3+).
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