Latest ArticlesCore-shell colloidal particles with a polymer layer have broad applications in different areas. Herein, we developed a two-step method combining aqueous surface-initiated photoinduced polymerization-induced self-assembly and photoinduced seeded reversible addition-fragmentation chain transfer (RAFT) polymerization to prepare a diverse set of core-shell colloidal particles with a well-defined polymer layer. Chemical compositions, structures, and thicknesses of polymer layers could be conveniently regulated by using different types of monomers and feed [monomer]/[chain transfer agent] ratios during seeded RAFT polymerization.
α-MnO2 is a potential positive electrode material for aqueous zinc-ion batteries, but its electrochemical performance of zinc storage requires further improvement. In this paper, potassium ion-doped manganese dioxide nanoscrolls (KMnO2) with oxygen vacancy were synthesized by a one-step hydrothermal method. It was observed that the electrochemical specific capacity was 250.9 mAh/g at a current density of 0.2 C, which was better than the existing commercial α-MnO2. At a high current of 1 C, these batteries demonstrate improved cycle stability. Synchrotron radiation and other experiments as well as DFT theoretical calculations provided additional evidence that K doping was efficient in regulating the metal bond type and the mean charge regulation of covalent bonds with oxygen atoms in MnO2. When MnO and MnK bonds are present, KMnO2 showed outstanding adsorption of Zn2+ and further enhanced the Zn2+ embedding process. Simultaneously, oxygen defects caused by doping boosted the development of the nanoscroll structure, leading to an increase in active sites available for electrochemical reactions and subsequently enhancing the electrical conductivity of α-MnO2. This study exhibits the potential of optimizing materials based on manganese with the introduction of a potassium doping strategy, resulting in improved performance for aquatic zinc-ion batteries, and presents novel perspectives for related research.
Carbonyl compounds are abundant in nature and represent a substantial portion of biomass resources. Despite significant recent progress in homo-coupling of carbonyl compounds, achieving their deoxy-functionalization homo-coupling remains a highly intricate challenge. Herein, we report an entirely novel reaction paradigm: the trifluoromethylative homo-coupling of carbonyl compounds via hydrazones, which enables the formation of three C(sp3)–C(sp3) bonds in a single step. This method provides a new pathway for synthesizing trifluoromethylative coupling product which has unique applications in both fields of medical and material sciences. Mechanistic investigations have unveiled that the formation of a trifluoromethyl-substituted benzyl radical plays a pivotal role as a key intermediate in this reaction.
Pure near-infrared (NIR) phosphorescent materials with emission peak larger than 700 nm are of great significance for the development of optoelectronics and biomedicine. We have designed and synthesized two new B-embedded pure near-infrared (NIR)-emitting iridium complexes (Ir(Bpiq)2acac and Ir(Bpiq)2dpm) with peaks greater than 720 nm. More importantly, they exhibit very narrow phosphorescent emission with full width at half maximum (FWHM) of only about 50 nm (0.12 eV), resulting in a high NIR content (> 90%) in their spectrum. In view of better optical property and solubility, the complex Ir(Bpiq)2dpm was used as the emitting layer of a solution-processed OLED device, and achieved good maximum external quantum efficiency (EQE) (2.8%) peaking at 728 nm. This research provides an important strategy for the design of narrowband NIR-emitting phosphorescent iridium complexes and their optoelectronic applications.
Designing highly active electrocatalysts for the hydrogen evolution reaction (HER) and oxygen evolution and reduction reactions (OER and ORR) is pivotal to renewable energy technology. Herein, based on density functional theory (DFT) calculations, we systematically investigate the catalytic activity of iron-nitrogen-carbon based covalent organic frameworks (COF) monolayers with axially coordinated ligands (denotes as FeN4-X@COF, X refers to axial ligand, X = -SCN, -I, -H, -SH, -NO2, -Br, -ClO, -Cl, -HCO3, -NO, -ClO2, -OH, -CN and -F). The calculated results demonstrate that all the catalysts possess good thermodynamic and electrochemical stabilities. The different ligands axially ligated to the Fe active center could induce changes in the charge of the Fe center, which further regulates the interaction strength between intermediates and catalysts that governs the catalytic activity. Importantly, FeN4-SH@COF and FeN4OH@COF are efficient bifunctional catalysts for HER and OER, FeN4OH@COF and FeN4-I@COF are promising bifunctional catalysts for OER and ORR. These findings not only reveal promising bifunctional HER/OER and OER/ORR catalysts but also provide theoretical guidance for designing optimum iron-nitrogen-carbon based catalysts.
As the global population ages, osteoporotic bone fractures leading to bone defects are increasingly becoming a significant challenge in the field of public health. Treating this disease faces many challenges, especially in the context of an imbalance between osteoblast and osteoclast activities. Therefore, the development of new biomaterials has become the key. This article reviews various design strategies and their advantages and disadvantages for biomaterials aimed at osteoporotic bone defects. Overall, current research progress indicates that innovative design, functionalization, and targeting of materials can significantly enhance bone regeneration under osteoporotic conditions. By comprehensively considering biocompatibility, mechanical properties, and bioactivity, these biomaterials can be further optimized, offering a range of choices and strategies for the repair of osteoporotic bone defects.
Heterodimerization in RTKs is of vital importance in the RTK signaling and cell functions. Heterodimerization between RTKs can result in diversity of downstream signals, increasing the ability of cells to respond to external experiments. Traditional RTKs heterodimerization always occur in the same families and is lack of agonists to activate the heterodimeric RTKs signaling pathway. Herein, we developed the DNA agonist based on bivalent aptamers for the heterodimerized RTKs of different families, AF/AM-1, which could simultaneously activate FGFR1 and c-Met signaling. It is the first agonist that realizing the heterodimerization and activation of FGFR1 and c-Met, two different RTK families. The activation of FGFR1/c-Met heterodimer result in the down-stream signals transduction, such as the phosphorylation of Akt and Erk, inducing the cell migration and proliferation. The DNA agonist for RTK heterodimer of different families would have potential applications in the fields of biomedicine.
Exploring transition metal sulfide electrocatalysts with high-efficiency for hydrogen evolution reaction (HER) is essential to produce H2 fuel through water splitting. Herein, novel nickel tungsten sulfide heterojunction (NiS-WS2) with a nanowoven ball-like structure were directed synthetized by a facile hydrothermal method. The hierarchical NiS-WS2 exhibited excellent HER activity with a relatively small overpotential of 142 and 137 mV at 10 mA/cm2 in 0.5 mol/L H2SO4 and 1 mol/L KOH, which is much better than that of single NiS and WS2. The impressive performance of NiS-WS2 heterojunction is owed to the collective synergy of special morphological and more exposed active sites between the crystal interfacial of NiS and WS2. In addition, the hierarchical NiS-WS2 can facilitate the transport of charge/mass by optimized electronic structure, which further improves the HER activity of electrocatalysts. These outcomes provide a simple method to prospect towards the design and application of heterostructures as efficient electrocatalysts, shedding some light on the development of functional materials in energy chemistry.
Multiple switchable physical channels within one material or device, encompassing optical, electrical, thermal, and mechanical pathways, can enable multifunctionality in mechanical-thermal-opto-electronic applications. Achieving integrated encryption and enhanced performance in storage and sensing presents a formidable challenge in the synthesis and functionality of new materials. In an effort to overcome the complexities associated with these multiple physical functions, this study investigates the large-size crystal of DPACdCl4 (DPA = diisopropylammonium), revealing significant features in rare multi-channel switches. This compound demonstrates the ability to switch between "OFF/0" and "ON/1" states in the mechanical-thermal-opto-electronic channels. Consequently, DPACdCl4 possesses four switchable physical channels, characterized by a higher phase transition temperature of 440.7 K and a competitive piezoelectric coefficient of 46 pC/N. Furthermore, solid-state NMR analysis indicates that thermally activated molecular vibrations significantly contribute to its multifunctional switching capabilities.
The first-ever synthesis of the unknown furo[2′,3′:4,5]pyrimido[1,2-b]indazole skeleton was demonstrated based on the undiscovered tetra-functionalization of enaminones, with simple substrates and reaction conditions. The key to realizing this process lies in the multiple trapping of the in situ generated ketenimine cation by the 3-aminoindazole, which results in the formation of four new chemical bonds and two new rings in one pot. Moreover, the products of this new reaction were found to exhibit aggregation-induced emission (AIE) without modification.
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