Latest ArticlesPhotocatalytic conversion of CO2 into small-molecule chemical feedstocks can meet the growing demand for energy and alleviate the global warming. Herein, a p-n ZnO@CDs@Co3O4 heterojunction with sandwich structure was constructed by calcination method of self-assembled ZIF-8@CDs@ZIF-67. The ZnO@CDs@Co3O4 with well-defined interfacial structure exhibited the significantly enhanced photocatalytic CO2 reduction activity, and the optimal catalyst indicated the (CO + CH4) evolution rate of 214.53 µmol g−1 h−1 under simulated solar light, which was superior to ZnO, Co3O4 and binary ZnO@Co3O4. The internal cavity, exposed active sites, multiple interfaces and constructed p-n heterojunction can facilitate the light harvesting and photoexcited electron transfer. Besides, after introduction of CDs placed in the middle layer between ZnO and Co3O4, CDs with excellent photoelectric property further promoted charge separation and migration. This work represents an appealing strategy to construct well-defined photocatalysts for boosting CO2 photoreduction.
Numerous supramolecular macrocycles have been utilized for developing catalysts by exploiting their specific molecular recognition and ability to form inclusion complexes through noncovalent interactions. The cyclic structure and modified functional groups of these macrocycles can influence substrate and transition state stability, as well as reaction selectivity. The inner cavities of these macrocycles are particularly beneficial, as they enable substrates to adopt preorganized arrangements and serve as versatile platforms for highly efficient supramolecular catalytic systems. This minireview provides an overview of recent advancements in supramolecular catalysis using various macrocycles, such as crown ethers, cyclodextrins, calixarenes, pillararenes, cucurbiturils, and other novel macrocycles.
Developing narrow-bandgap organic semiconductors is important to facilitate the advancement of organic photovoltaics (OPVs). Herein, two near-infrared non-fused ring acceptors (NIR NFRAs), PTBFTT-F and PTBFTT-Cl have been developed with A-πA-πD-D-πD-πA-A non-fused structures. It is revealed that the introduction of electron deficient π-bridge (πA) and multiple intramolecular noncovalent interactions effectively retained the structural planarity and intramolecular charge transfer of NFRAs, extending strong NIR photon absorption up to 950 nm. Further, the chlorinated acceptor, with the enlarged π-surface compared to the fluorinated counterpart, promoted not only molecular stacking in solid, but also the desirable photochemical stability in ambient, which are helpful to thereby improve the exciton and charge dynamics for the corresponding OPVs. Overall, this work provides valuable insights into the design of NIR organic semiconductors.
While heteroatom doping serves as a powerful strategy for devising novel polycyclic aromatic hydrocarbons (PAHs), the further fine-tuning of optoelectronic properties via the precisely altering of doping patterns remains a challenge. Herein, by changing the doping positions of heteroatoms in a diindenopyrene skeleton, we report two isomeric boron, sulfur-embedded PAHs, named Anti-B2S2 and Syn-B2S2, as electron transporting semiconductors. Detailed structure-property relationship studies revealed that the varied heteroatom positions not only change their physicochemical properties, but also largely affect their solid-state packing modes and Lewis base-triggered photophysical responses. With their low-lying frontier molecular orbital levels, n-type characteristics with electron mobilities up to 1.5 × 10−3 cm2 V−1 s−1 were achieved in solution-processed organic field-effect transistors. Our work revealed the critical role of controlling heteroatom doping patterns for designing advanced PAHs.
Single-emitter white organic light-emitting diode (WOLED) based on small organic molecule exhibits great potential in simplifying fabrication process of WOLEDs. However, the design and synthesis of molecule for highly efficient single-emitter WOLED still remains a challenge. Herein, two asymmetric donor-acceptor-acceptor' (D-A-A') type molecule (PTZ-PQ-F and PTZ-PQ-CF3) are developed by employing trifluoromethyl (CF3) or fluorine atom as secondary acceptor, which can exhibit white lighting with dual emission bands consisting of blue traditional fluorescence from quasi-axial (ax) conformer and orange thermally activated delayed fluorescence (TADF) from quasi-equatorial (eq) conformer. The introduction of CF3 into PTZ-PQ-CF3 greatly enhanced the photoluminescence quantum yield (PLQY) by suppressing the nonradiative deactivation. Owing to electron-inductive-effect of CF3, the "eq" conformer of PTZ-PQ-CF3 exhibits a much smaller ΔEST of 0.01 eV to realize more efficient reverse intersystem crossing (RISC) process, and then enhance the exciton utilization (nearly 100%) of the whole dual emission system. Consequently, single-emitter WOLEDs based on PTZ-PQ-CF3 show nearly standard white emission with EQE of 13.0% and CIE of (0.35, 0.36) in mCP host and show warm white emission with high EQE of 25.5% and CIE of (0.40, 0.47) in 35 DczPPy host, which are the best performance among reported single-emitter WOLEDs.
Aging is a natural physiological process with various challenges, related to the loss of homeostasis within the organism, which is not a disease, but a significantly strong risk factor for multiple diseases, including myocardial infarction, stroke, some age-related cancers, macular degeneration, osteoarthritis, neurodegeneration, and many others. In the body, the main manifestation of aging is cellular aging, which exists within tissues and has a local or global impact on tissue function. However, the lack of effective aging detection tools has always been an issue that cannot be ignored in the field of aging research. Therefore, it is necessary to construct a non-invasive tool for in vivo detection of aging. Here, we show that the photoacoustic probe (LGAL), which has peak excitation and emission wavelengths in the near-infrared optical window, binds in vivo and at high contrast to the hallmark of aging, and allows for the microscopic imaging of aging through the intact mice. Firstly, this tool LGAL has been successfully applied to detect senescence in cells, displaying stronger photoacoustic signals than normal cells. Then, by using the photoacoustic probe, the blood vessels and tissues inside the mice can be visualized. Young and elderly mice exhibit varying intensities of photoacoustic signals, marking the first time a probe has been used to explore the aging of blood vessels and tissues inside the mice. Finally, we monitored the changes in the degree of aging during tumor treatment under photoacoustic (PA) imaging for the first time. As the treatment time increased, the degree of aging of the tumor gradually deepened. We expect the powerful tool could be a noninvasive and powerful tool for the study of aging biology.
The photovoltaic properties of double-cable conjugated polymers are significantly influenced by the length of the alkyl linkers that connect donor backbones and acceptor side units. In this study, a series of 2-(3-oxo-2,3-dihydroinden-1-ylidene)malononitrile (IC)-based double-cable polymers with alkyl linkers ranging from C8H16 to C16H32 (Px, x = 8, 10, 12, 14, 16) were synthesized for single-component organic solar cells (SCOSCs). Among these, the linker length x = 12 (P12) is found to optimize the power conversion efficiencies (PCEs) in SCOSCs. Specifically, PCEs increase from P8 to P12 and then decline from P12 to P16. Detailed investigations of optical absorption, charge transport, and morphology provide insights into the underlying factors contributing to these PCE variations. The findings indicate that the exceptional photovoltaic properties observed in P12 can be attributed to three key factors: A delicate balance between enhanced charge separation facilitated by the increased spacer length and reduced crystallinity resulting from longer spacers, higher charge mobilities, and well-balanced hole/electron transport characteristics. This study highlights the critical role of linker length in determining the photovoltaic properties of double-cable conjugated polymer-based SCOSCs and offers valuable guidance for the design of novel double-cable conjugated polymers.
Cultural relics have their unique artistic, cultural and historical value, and the protection of important cultural relics is conducive to the inheritance of historical culture. As a kind of cementing agent and binder commonly seen in cultural relics protection, epoxy resin is widely used in the bonding and consolidation of various materials in cultural relics, which has important practical application value. In this review, a systematic classification of commonly used epoxy resins, including their molecular structures, synthesis reactions and properties are provided, the problems and solutions of epoxy resin in cultural relics protection are summarized. The solutions are classified into three aspects: functional epoxy resin, blending modification, and other modification. Representative application examples of epoxy resin are listed in the field of cultural relics protection, and the development direction of epoxy resin in cultural relics protection in the future is proposed, which provides useful guidance for the modification of epoxy resin and its application in cultural relics protection in the future.
Application of transition metal boride (TMB) catalysts towards hydrolysis of NaBH4 holds great significance to help relieve the energy crisis. Herein, we present a facile and versatile metal-organic framework (MOF) assisted strategy to prepare Co2B-CoPOx with massive boron vacancies by introducing phytic acid (PA) cross-linked Co complexes that are acquired from reaction of PA and ZIF-67 into cobalt boride. The PA etching effectively breaks down the structure of ZIF-67 to create more vacancies, favoring the maximal exposure of active sites and elevation of catalytic activity. Experimental results demonstrate a drastic electronic interaction between Co and the dopant phosphorous (P), thereby the robustly electronegative P induces electron redistribution around the metal species, which facilitates the dissociation of B-H bond and the adsorption of H2O molecules. The vacancy-rich Co2B-CoPOx catalyst exhibits scalable performance, characterized by a high hydrogen generation rate (HGR) of 7716.7 mL min−1 g−1 and a low activation energy (Ea) of 44.9 kJ/mol, rivaling state-of-the-art catalysts. This work provides valuable insights for the development of advanced catalysts through P doping and boron vacancy engineering and the design of efficient and sustainable energy conversion systems.
In an era where the concept of green development is deeply rooted, magnesium (Mg) alloy as a light metal has a long-term development prospect in the process of energy saving, emission reduction and environmental improvement. However, anti-corrosion performance of Mg alloy is poor due to the high chemical activity and low equilibrium potential, which limits the development of Mg alloy products. Herein, three-dimensional mesopore hollow polypyrrole spheres (MHPS) were prepared, and the MHPS was inserted into the middle of the stacked hexagon boron nitride (h-BN) lamellae, which allowed the h-BN to be separated forming a further composite with abundant pore structure. Subsequently, the MHPS/h-BN-OH composite was uniformly sprayed on the Mg alloy surface via simple spraying method to form the superhydrophobic surface (SHS). Finally, the slippery liquid infused porous surface (SLIPS) was successfully fabricated by applying drops of silicone lubricant on the superhydrophobic coating surface. After a series of characterization and testing, the results showed that the stacking of h-BN lamellae was significantly reduced after h-BN was successfully embedded by MHPS. In addition, the fabricated SLIPS have excellent self-cleaning, mechanical stability, anti-icing and anti-corrosion properties. Therefore, the method of embedding polymer microspheres not only offers a new strategy for h-BN exfoliation, but also the successful prepared SLIPS largely retards the corrosion of Mg alloy while providing new ideas for the development of SLIPS.
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