Latest ArticlesPhotoinitiators (PIs), as the key substances for photopolymerized antibacterial film (PAF), affect the cure rate and color of PAF. Herein, two enone dyes were designed and synthesized by a facile approach. Among the candidates, BDO1 has demonstrated the ability to initiate polymerization of acrylate monomers as single-component PI with the advantages of low mobility, outstanding photobleaching, excellent cytocompatibility, and suitability for light emitting diode (LED) light sources above 365 nm. Taking BDOs as examples, a novel method based on theoretical calculations aiming to assess the potential of enone molecules as single-component PIs was proposed. Finally, under the initiation of BDO1, tannic acid was photopolymerized to a colorless and transparent antibacterial film with high antibacterial ability, which indicated that BDO1 was expected to be used in environmentally friendly PAF.
Polyphosphazene with phenoxy or 4-ester phenoxy as pendent groups are demonstrated as both ligands and host matrices for CsPbBr3 perovskite nanocrystals (NCs). These polymers produced flexible nanocomposite films with excellent NCs dispersion, optical transparency and stability in various extreme conditions. Both films remained stable even after 30 days of air storage. CsPbBr3/poly[bis(phenoxy phosphazene)] (PBPP) delivered better air and light stability, and CsPbBr3/poly[bis(4-esterphenoxy)phosphazene] (PBEPP) exhibited superior water and heat resistance. CsPbBr3/PBEPP showed a greater increase in fluorescence intensity under 365 nm UV light and demonstrated a 10% luminescence increase after 96 h of water immersion and even at high temperature (150 ℃). These findings thus provide new insight into flexible luminescent CsPbBr3 films with high stability in optoelectronic applications.
Enhancement of the nonlinear optical (NLO) output power of lasers requires urgent development of an NLO crystal with a significant second-harmonic generation (SHG) response and sufficient birefringence for phase-matching capability; however, simultaneously optimizing these two key parameters remains a great challenge. In contrast to traditional single-anion units, the stereochemically-active lone pair Sb3+ ion is coordinated by S2− and I− ions to yield the mixed-anionic SbSI chalcohalide that can enhance hyperpolarizability and anisotropic polarizability concurrently. As anticipated, SbSI exhibited the largest SHG response (5.7 × AgGaS2@1.91 µm) among phase-matching Sb-based sulfides, the favorable laser-induced damage threshold (LIDT, 2.3 × AgGaS2@2.09 µm), and the giant calculated birefringence (0.62@1.91 µm). Structural analysis and computational simulations indicate that the highly polarizable mixed anion determine the enormous SHG response and birefringence.
Heterogeneous metal-catalyzed chemical conversions with a recyclable catalyst are very ideal and challenging for sustainable organic synthesis. A new bipyridyl-Mo(Ⅳ)-carbon nitride (CN-K/Mo-Bpy) was prepared by supporting molybdenum complex on C3N4-K and characterized by FT-IR, XRD, SEM, XPS and ICP-OES. Heterogeneous CN–Mo-Bpy catalyst can be applied to the direct amination of nitroarenes and arylboronic acid, thus constructing various valuable diarylamines in high to excellent yields with a wide substrate scope and good functional group tolerance. It is worth noting that this heterogeneous catalyst has high chemical stability and can be recycled for at least five times without reducing its activity.
The utilization of ethane-selective materials for adsorption-based separation technology presents an energy-efficient alternative to cryogenic distillation for ethylene (C2H4) purification from ethane (C2H6). To study the relations between separation performance and pore environments, we carried out the isoreticular chemistry rule to introduce the -NH2 groups into a C2H6-selective MOF [Cu1.5(BTC)(DPU)1.5(H2O)1.5], and successfully improved the adsorption capacity and selectivity for C2H6 over C2H4. The NH2-functionalized MOF [Cu1.5(NH2-BTC)(DPU)1.5(H2O)1.5] with a relatively narrow pore not only forms appropriate pore restriction but also provides additional binding sites to enhance the adsorption capacity of C2H6 relative to C2H4. Both gas adsorption and dynamic breakthrough results indicated that the -NH2 functionalization significantly enhanced the separation performance of materials for C2H6/C2H4 mixtures, allowing the production of C2H4 with a purity of over 99.99% and a productivity of up to 30.02 L/kg in one step. Theoretical calculations revealed that the synergistic effect of appropriate pore confinement and NH2-modified functional surfaces imposed stronger interactions on C2H6 than C2H4.
Glial fibrillary acidic protein (GFAP) is one of the discriminative biomarkers for diagnosing traumatic brain injury (TBI), and accurate determination of GFAP is clinically significant. In this study, a novel fluorescence immunoassay system was designed. We encapsulated carbon dots with a high fluorescence quantum yield (QY = 92.5%) inside silicon nanocapsules to serve as fluorescent markers. These markers were then integrated with the streptavidin (SA)-biotin biomagnification system and immunomagnetic separation technology for the sensitive detection of GFAP. Based on the signal cascade amplification effect of the silicon nanocapsules and SA-biotin, the fluorescence signal of the SA-biotin-modified immunofluorescence nanocapsules increased 3.6-fold compared to the carbon dot-based immunoprobe. The fluorescence immunoassay system was constructed for GFAP using SA-biotin-modified immunocapsules as the sensing probe and immunomagnetic nanoparticles as the immunorecognition probe. The fluorescence immunoassay system can specifically and ultra-sensitively quantify GFAP in blood samples, with a detection range of 10 pg/mL–10 ng/mL and detection limits of 3.2 pg/mL (serum) and 3.6 pg/mL (plasma). Moreover, the fluorescence immunoassay system exhibited prominent recoveries of 99.4%–100.4% (phosphate buffered saline), 96%–102.6% (serum), and 93.2%–110.2% (plasma), with favorable specificity and excellent stabilization. The novel fluorescence immunoassay system provides a new approach to the clinical analysis of GFAP and may serve as a potential tool for screening and diagnosing TBI.
Deprivation of glucose and lactate provides an effective pathway to terminate the nutrients supplement for tumor growth. In this work, biomimetic nanozymes called m@BGLC are constructed for catalytic tumor inhibition through nutrients deprivation and oxidative damage induction. Concretely, the catalytic enzymes of glucose oxidase (GOx), lactate oxidase (LOx) and chloroperoxidase (CPO) are precrosslinked with bovine serum albumin (BSA) to construct nanozymes, which are then biomimetic functionalized with cancer cell membrane to prepare m@BGLC. Benefiting from the biomimetic camouflage with homologous cell membrane, m@BGLC inherit homotypic binding and immune escape abilities, facilitating the tumor targeting accumulation and preferable cell internalization for improved drug delivery efficiency. Subsequently, under the cascade catalysis of nanozymes, m@BGLC consume glucose and lactate for tumor starvation therapy through nutrients deprivation, and meanwhile, the resulting hyprochloric acid (HClO) causes an oxidative damage of cells to synergistically inhibit tumor growth. In vitro and in vivo findings demonstrate a robust tumor eradication effect of m@BGLC without obvious adverse reactions via the targeted combination therapy. Such cascade catalytic nanomedicine may inspire the development of sophisticated strategies for tumor combination therapy under unfavorable tumor microenvironments.
In the field of Raman spectroscopy detection, the quest for a non–noble metal, recyclable, and highly sensitive detection substrate is of utmost importance. In this work, a new crystalline and noble metal–free substrate of [Bi(DMF)8][PMo12O40] (Bi–PMo12) is designed, which is composed of [PMo12O40]3− and solvated [Bi(DMF)8]3+ cations. Mechanistic studies have revealed that Raman scattering quenching phenomenon arises from two main factors. Firstly, it arises from the absorption of the scattered light due to the transition of a single electron in the reduced state of MoV between 4d orbitals. Secondly, after the interaction between the substrate and hydrazine, the surface undergoes varying degrees of roughening, leading to an impact on the scattered light intensity. These two effects collectively contribute to the detection of low concentrations of N2H4. As a result, Bi–PMo12 opens up a novel Raman scattering quenching mechanism to realize the detection of reduced N2H4 small molecules. A remarkably low detection limit of 4.5 × 10−9 ppm for N2H4 is achieved on the Bi–PMo12 substrate. This detection has a lower concentration than the currently known SERS detection of N2H4. Moreover, Bi–PMo12 can be recovered and reused through recrystallization, achieving a recovery rate of up to ca. 51%. This study reveals the underlying potential of crystalline polyoxometalate materials in the field of Raman detection, thus opening up new avenues for highly sensitive analysis using Raman techniques.
The performance optimization of materials is an eternal theme and challenge in scientific research, which is reflected in ferroelectric filed to two hot topics of enhancing Curie temperature (TC) and functional versatility. The former one vitally determines ferroelectric operational temperature range while the latter would open up new application possibilities. Effective chemical modification or doping strategies on A-site and X-site components have been successfully developed in hybrid organic-inorganic perovskite (HOIP) ferroelectrics, however, the important role of adjusting B-site ions has long been overlooked. Here, we have implemented regulation on the ion radius of the B-site component to successfully obtain two new HOIP ferroelectrics (3-pyrrolinium)BBr3 (B = Mn and Ni). Compared to parent (3-pyrrolinium)CdBr3, the TC (ΔT = 99 K) was significantly optimized by replacing the Cd2+ with smaller Mn2+ or Ni2+ ions. More strikingly, the introduction of Mn2+ and Ni2+ ions with octahedral coordination bring out intriguing red emission and magnetism respectively, making the multifunctional integration in a single material for multiple uses. This work provides a feasible strategy for performance optimizing of HOIP ferroelectrics, and would shed light for constructing multifunctional ferroelectrics.
Herein, we developed the first example of copper-catalyzed silicon radical-initiated 1,4-silylcyanation of unactivated 1,3-enynes, which provided an efficient method to access CN-bearing tri- and tetra-substituted homoallenylsilane derivatives in high yields with excellent regioselectivities. This protocol featured good functional group compatibility and broad substrate scopes, enabling the formation of C-Si bond under cheap copper catalyst with a low loading. Furthermore, this means showed potential application value in the late-stage functionalization of natural products.
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