Organic cocrystals based on noncovalent intermolecular interactions (weak interactions) have aroused interest owing to their unpredicted and versatile chemicophysical properties and their applications. In this Minireview, we highlight recent research on organic cocrystals on reducing the aggregation‐caused quenching (ACQ) effect, tuning light emission, ferroelectricity and multiferroics, optical waveguides, and stimuli‐responsiveness. We also summarize the progress made in this field including revealing the structure–property relationships and developing unusual properties. Moreover, we provide a discussion on current achievements, limitations and perspectives as well as some directions and inspiration for further investigation on organic cocrystals.
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.
Membranes for organic solvent nanofiltration (OSN) or solvent-resistant nanofiltration (SRNF) offer unprecedented opportunities for highly efficient and cost-competitive solvent recovery in the pharmaceutical industry. Here, we describe small-flake graphene oxide (SFGO) membranes for high-performance OSN applications. Our strategy exploits lateral dimension control to engineer shorter and less tortuous transport pathways for solvent molecules. By using La3+ as a cross-linker and spacer for intercalation, the SFGO membrane selective layer was stabilized, and size-dependent ultrafast selective molecular transport was achieved. The methanol permeance was up to 2.9-fold higher than its large-flake GO (LFGO) counterpart, with high selectivity toward three organic dyes. More importantly, the SFGO-La3+ membrane demonstrated robust stability for at least 24 hours under hydrodynamic stresses that are representative of realistic OSN operating conditions. These desirable attributes stem from the La3+ cross-linking, which forms uniquely strong coordination bonds with oxygen-containing functional groups of SFGO. Other cations were found to be ineffective.
Aqueous rechargeable zinc‐ion batteries (ZIBs) have attracted considerable attention as a promising candidate for low‐cost and high‐safety electrochemical energy storage. However, the advancement of ZIBs is strongly hindered by the sluggish ionic diffusion and structural instability of inorganic metal oxide cathode materials during the Zn2+ insertion/extraction. To address these issues, a new organic host material, poly(2,5‐dihydroxy‐1,4‐benzoquinonyl sulfide) (PDBS), has been designed and applied for zinc ion storage due to its elastic structural factors (tunable space and soft lattice). The aqueous Zn‐organic batteries based on the PDBS cathode show outstanding cycling stability and rate capability. The coordination moieties (O and S) display the strong electron donor character during the discharging process and can act as the coordination arms to host Zn2+. Also, under the electrochemical environment, the malleable polymer structure of PDBS permits the rotation and bending of polymer chains to facilitate the insertion/extraction of Zn2+, manifesting the superiority and uniqueness of organic electrode materials in the polyvalent cation storage. Finally, quasi‐solid‐state batteries based on aqueous gel electrolyte demonstrate highly stable capacity under different bending conditions.
Structurally well-defined graphene nanoribbons (GNRs) have attracted great interest as next-generation semiconductor materials. The functionalization of GNRs with polymeric side chains, which can widely broaden GNR-related studies on physiochemical properties and potential applications, has remained unexplored. Here, we demonstrate the bottom-up solution synthesis of defect-free GNRs grafted with flexible poly(ethylene oxide) (PEO) chains. The GNR backbones possess an armchair edge structure with a width of 1.0-1.7 nm and mean lengths of 15-60 nm, enabling near-infrared absorption and a low bandgap of 1.3 eV. Remarkably, the PEO grafting renders the GNRs superb dispersibility in common organic solvents, with a record concentration of ∼1 mg mL(-1) (for GNR backbone) that is much higher than that (<0.01 mg mL(-1)) of reported GNRs. Moreover, the PEO-functionalized GNRs can be readily dispersed in water, accompanying with supramolecular helical nanowire formation. Scanning probe microscopy reveals raft-like self-assembled monolayers of uniform GNRs on graphite substrates. Thin-film-based field-effect transistors (FETs) of the GNRs exhibit a high carrier mobility of ∼0.3 cm(2) V(-1) s(-1), manifesting promising application of the polymer-functionalized GNRs in electronic devices.
We present a novel type of "rod-coil" graft copolymer containing a polyphenylene backbone linked with poly(ethylene oxide) (PEO) side chains. Such graft copolymers manifest unprecedented temperature-dependent one-dimensional (1D) and two-dimensional (2D) self-assembly in solution. At 20 °C, which is higher than the crystallization temperature (Tc) of the PEO chains, the achiral graft copolymers self-organize into nanoribbons that twist into ∼30 μm ultralong helices with controlled pitch depending on the grafting ratio of the PEO chains. At 10 °C, which is lower than the Tc, quadrangular multilayer sheets of over 10 μm in lateral size are obtained. To our knowledge, this work presents the first example of controlled self-assembly of graft polymers into 1D helix and 2D sheet superstructures.
We report a novel type of structurally defined graphene nanoribbons (GNRs) with uniform width of 1.7 nm and average length up to 58 nm. These GNRs are decorated with pending Diels-Alder cycloadducts of anthracenyl units and N- n-hexadecyl maleimide. The resultant bulky side groups on GNRs afford excellent dispersibility with concentrations of up to 5 mg mL in many organic solvents such as tetrahydrofuran (THF), two orders of magnitude higher than the previously reported GNRs. Multiple spectroscopic studies confirm that dilute dispersions in THF (<0.1 mg mL) consist mainly of nonaggregated ribbons, exhibiting near-infrared emission with high quantum yield (9.1%) and long lifetime (8.7 ns). This unprecedented dispersibility allows resolving in real-time ultrafast excited-state dynamics of the GNRs, which displays features of small isolated molecules in solution. This study achieves a breakthrough in the dispersion of GNRs, which opens the door for unveiling obstructed GNR-based physical properties and potential applications.
This study reports an environment-friendly waterborne hydrophobic bio-epoxy coating (WHBC), prepared by introducing dual-scale SiO2 nanoparticles and (3-Glycidyloxypropyl) trimethoxysilane into an aqueous mixture containing the isosorbide based epoxy and a hydrophobic curing agent. The coatings were applied on Fe foil substrates using a one-step spin-coating method. The optimal coating with 33.3 wt.% SiO2 nanoparticles exhibits high hydrophobicity with a water contact angle (CA) of 153.0 ± 1.1° and a sliding angle (SA) of 14.3 ± 1.9°. This optimal coating is found to have good mechanical durability against sand erosion.It maintained a high CA of 151.3 ± 2.0° and increased SA of 23.4 ± 3.7° after mechanical sandblasting for 30 s. The as-prepared optimal coating also showed excellent self-cleaning performance and was able to retain the good self-cleaning ability after the sandblasting. In addition, the as-obtained optimal coating shows a much lower icing temperature, a significantly longer icing delay time, and a low ice adhesion strength at 0.101 ± 0.019 MPa. The developed coating is biobased and green, which holds various promising applications for marine, aerospace, energy harvesting and sports applications.
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