3D carbon superstructures are fabricated through the hierarchical assembly of polyimide nanosheets and thermal treatment. Benefiting from the ultrahigh surface area and the hierarchically porous structure, along with the well-distributed highly electroactive sites, the flower-like carbon material exhibits outstanding catalytic activity toward the oxygen reduction reaction and also serves as a highly stable electrode material in supercapacitors.
Two new crystalline covalent organic frameworks are synthesized and structure modulated as high rate and stable cathode materials for Li-ion batteries.
The discovery of the striking aggregation-induced emission (AIE) phenomenon has opened a new avenue for smart light-emitting materials. Herein, a new AIE luminogen (AIEgen), 1,1,2,2-tetrakis(4-((E)-2-(pyridin-2-yl)vinyl)phenyl)ethene (TP2VPE), has been designed and synthesized by introducing the vinylpyridine motifs into the tetraphenylethene backbone. The emission spectrum of the new obtained AIEgen crystalline material can be switched in response to not only mechanical grinding and hydrostatic compression but also the protonation effect with excellent reversibility and reproducibility. Single-crystal X-ray structural analysis disclosed the supramolecular porous channel structure, which provides a shrinkable volume to maintain the fluorescence emission upon high pressure. Furthermore, protonation-deprotonation of the pyridine moieties in TP2VPE has a significant effect on the frontier molecular orbitals as well as very distinctive emission characteristics upon acid and base stimuli. The dual-response performance and the ease of its preparation and renewal endow the material with potential applications in pressure and acid/alkali fluorescence sensing.
Among the rising 2D soft materials, conjugated polymer nanosheets are one of the most promising and new classes of polymeric materials, which are rarely developed because of the challenge in controlling the dimensionality and lack of synthetic strategies. In this study, one kind of sulfur‐enriched conjugated polymer nanosheet (2DP‐S) with a high aspect ratio of up to ≈400 is successfully synthesized. On the basis of structural characterization, as‐prepared 2DP‐S possesses the chemical identity of cruciform‐fused polymeric backbone consisting of quinoidal polythiophene and poly(p‐phenylenevinylene) along horizontal and vertical directions, respectively, by sharing two alternating single–double carbon–carbon bonds in each repeat unit. The unique structural conformation of 2DP‐S renders carrier mobilities of up to 0.1 ± 0.05 cm2 V−1 s−1, a figure inferred from Terahertz time domain spectroscopy. Moreover, upon thermal treatment, 2DP‐S is readily converted into N/S dual‐doped porous carbon nanosheets (2DPCs) under ammonia atmosphere, whose N/S ratio can be rationally controlled by adjusting the activation time. The catalytic performance of the oxygen reduction reaction of as‐prepared 2DPCs is well tunable by the rationally controlled N/S contents. These results offer a new pathway for exploring heteroatom‐doped porous carbons applicable for energy conversion and storage.
A novel phosphorus‐containing porous polymer is efficiently prepared from tris(4‐vinylphenyl)phosphane by radical polymerization, and it can be easily ionized to form an ionic porous polymer after treatment with hydrogen iodide. Upon ionic exchange, transition‐metal‐containing anions, such as tetrathiomolybdate (MoS4
2−) and hexacyanoferrate (Fe(CN)6
3−), are successfully loaded into the framework of the porous polymer to replace the original iodide anions, resulting in a polymer framework containing complex anions (termed HT‐Met, where Met = Mo or Fe). After pyrolysis under a hydrogen atmosphere, the HT‐Met materials are efficiently converted at a large scale to metal‐phosphide‐containing porous carbons (denoted as MetP@PC, where again Met = Mo or Fe). This approach provides a convenient pathway to the controlled preparation of metal‐phosphide‐loaded porous carbon composites. The MetP@PC composites exhibit superior electrocatalytic activity for the hydrogen evolution reaction (HER) under acidic conditions. In particular, MoP@PC with a low loading of 0.24 mg cm−2 (on a glass carbon electrode) affords an iR‐corrected (where i is current and R is resistance) current density of up to 10 mA cm−2 at 51 mV versus the reversible hydrogen electrode and a very low Tafel slope of 45 mV dec−1, in rotating disk measurements under saturated N2 conditions.
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