Latest ArticlesA phenylphenothiazine anchored Tb(Ⅲ)-cyclen complex PTP-Cy-Tb for hypochlorite ion (ClO−) detection has been designed and prepared. PTP-Cy-Tb shows a weak Tb-based emission with AIE-characteristics in aqueous solutions. After addition of ClO−, the fluorescence of PTP-Cy-Tb gives a large enhancement for oxidization the thioether to sulfoxide group. The detection limit of PTP-Cy-Tb toward ClO− is as low as 8.85 nmol/L. The sensing mechanism was detailedly investigated by time of flight mass spectrometer (TOF-MS), Fourier transform infrared spectroscopy (FT-IR) and density functional theory (DFT) calculation. In addition, PTP-Cy-Tb has been successfully used for on-site and real-time detection of ClO− in real water samples by using the smartphone-based visualization method and test strips.
Propane dehydrogenation (PDH) is a vital industrial process for producing propene, utilizing primarily Cr-based or Pt-based catalysts. These catalysts often suffer from challenges such as the toxicity of Cr, the high costs of noble metals like Pt, and deactivation issues due to sintering or coke formation at elevated temperatures. We introduce an exceptional Ru-based catalyst, Ru nanoparticles anchored on a nitrogen-doped carbon matrix (Ru@NC), which achieves a propane conversion rate of 32.2% and a propene selectivity of 93.1% at 550 ℃, with minimal coke deposition and a low deactivation rate of 0.0065 h−1. Characterizations using techniques like TEM and XPS, along with carefully-designed controlled experiments, reveal that the notable performance of Ru@NC stems from the modified electronic state of Ru by nitrogen dopant and the microporous nature of the matrix, positioning it as a top contender among state-of-the-art PDH catalysts.
Lithium-ion batteries (LiBs) with high energy density have gained significant popularity in smart grids and portable electronics. LiMn1-xFexPO4 (LMFP) is considered a leading candidate for the cathode, with the potential to combine the low cost of LiFePO4 (LFP) with the high theoretical energy density of LiMnPO4 (LMP). However, quantitative investigation of the intricate coupling between the Fe/Mn ratio and the resulting energy density is challenging due to the parametric complexity. It is crucial to develop a universal approach for the rapid construction of multi-parameter mapping. In this work, we propose an active learning-guided high-throughput workflow for quantitatively predicting the Fe/Mn ratio and the energy density mapping of LMFP. An optimal composition (LiMn0.66Fe0.34PO4) was effectively screened from 81 cathode materials via only 5 samples. Model-guided electrochemical analysis revealed a nonlinear relationship between the Fe/Mn ratio and electrochemical properties, including ion mobility and impedance, elucidating the quantitative chemical composition-energy density map of LMFP. The results demonstrated the efficacy of the method in high-throughput screening of LiBs cathode materials.
It is well known that cationic polymers have excellent antimicrobial capacity accompanied with high biotoxicity, to reduce biotoxicity needs to decrease the number of cationic groups on polymers, which will influence antimicrobial activity. It is necessary to design a cationic polymer mimic natural antimicrobial peptide with excellent antibacterial activity and low toxicity to solve the above dilemma. Here, we designed and prepared a series of cationic poly(β-amino ester)s (PBAEs) with different cationic contents, and introducing hydrophobic alkyl chain to adjust the balance between antimicrobial activity and biotoxicity to obtain an ideal antimicrobial polymer. The optimum one of synthesized PBAE (hydrophilic cationic monomer: hydrophobic monomer = 5:5) was screened by testing cytotoxicity and minimum inhibitory concentration (MIC), which can effectively kill S. aureus and E. coli with PBAE concentration of 15 µg/mL by a spread plate bacteriostatic method and dead and alive staining test. The way of PBAE killing bacterial was destroying the membrane like natural antimicrobial peptide observed by scanning electron microscopy (SEM). In addition, PBAE did not exhibit hemolysis and cytotoxicity. In particular, from the result of animal tests, the PBAE was able to promote healing of infected wounds from removing mature S. aureus and E. coli on the surface of infected wound. As a result, our work offers a viable approach for designing antimicrobial materials, highlighting the significant potential of PBAE polymers in the field of biomedical materials.
The detrimental phase transformations of sodium layered transition metal oxides (NaxTMO2) during desodiation/sodiation seriously suppress their practical applications for sodium ion batteries (SIBs). Undoubtedly, comprehensively investigating of the dynamic crystal structure evolutions of NaxTMO2 associating with Na ions extraction/intercalation and then deeply understanding of the relationships between electrochemical performances and phase structures drawing support from advanced characterization techniques are indispensable. In-situ high-energy X-ray diffraction (HEXRD), a powerful technology to distinguish the crystal structure of electrode materials, has been widely used to identify the phase evolutions of NaxTMO2 and then profoundly revealed the electrochemical reaction processes. In this review, we begin with the descriptions of synchrotron characterization techniques and then present the advantages of synchrotron X-ray diffraction (XRD) over conventional XRD in detail. The optimizations of structural stability and electrochemical properties for P2-, O3-, and P2/O3-type NaxTMO2 cathodes through single/dual-site substitution, high-entropy design, phase composition regulation, and surface engineering are summarized. The dynamic crystal structure evolutions of NaxTMO2 polytypes during Na ion extraction/intercalation as well as corresponding structural enhancement mechanisms characterizing by means of HEXRD are concluded. The interior relationships between structure/component of NaxTMO2 polytypes and their electrochemical properties are discussed. Finally, we look forward the research directions and issues in the route to improve the electrochemical properties of NaxTMO2 cathodes for SIBs in the future and the combined utilizations of multiple characterization techniques. This review will provide significant guidelines for rational designs of high-performance NaxTMO2 cathodes.
The photoinduced ligand-to-metal charge transfer (LMCT) process has been extensively investigated, however, the recovery of photocatalysts has remained a persistent challenge in the field. In light of this issue, a novel approach involving the development of iron-based ionic liquids as photocatalysts has been pursued for the first time, with the goal of simultaneously facilitating the LMCT process and addressing the issue of photocatalyst recovery. Remarkably, the iron-based ionic liquid 1-butyl-3-methylimidazolium tetrachloroferrate (C4mim-FeCl4) demonstrates exceptional recyclability and stability for the photocatalytic hydroacylation of olefins. This study will pave the way for new approaches to photocatalytic organic synthesis using ionic liquids as recyclable photocatalysts.
This work develops a protein imprinted nanosphere with varied recognition specificity for bovine serum albumin (BSA) and lysozyme (Lyz) under different UV light through a gradient dual crosslinked imprinting strategy (i.e., covalent crosslinking and dynamic reversible crosslinking). The imprinting cavities are initially constructed using irreversible covalent crosslinking to specifically recognize BSA, and then the coumarin residues in the imprinting cavities are crosslinked under 365 nm UV light to further imprint Lyz, because Lyz has smaller size than BSA. Since the photo-crosslinking of coumarin is a reversible reaction, the imprinting cavities of Lyz can be de-crosslinked under 254 nm UV light and restore the imprinting cavities of BSA. Moreover, the N-isopropyl acrylamide (NIPAM) and pyrrolidine residues copolymerized in the polymeric surface of the nanospheres are temperature- and pH-responsive respectively. Therefore, the protein rebinding and release behaviors of the nanospheres are controlled by external temperature and pH. As a result, the materials can selectively separate BSA from real bovine whole blood and Lyz from egg white under different UV light. This study may provide a new strategy for construction of protein imprinted materials with tunable specificity for different proteins.
Solar-induced water oxidation reaction (WOR) for oxygen evolution is a critical step in the transformation of Earth’s atmosphere from a reducing to an oxidation one during its primordial stages. WOR is also associated with important reduction reactions, such as oxygen reduction reaction (ORR), which leads to the production of hydrogen peroxide (H2O2). These transitions are instrumental in the emergence and evolution of life. In this study, transition metals were loaded onto nitrogen-doped carbon (NDC) prepared under the primitive Earth’s atmospheric conditions. These metal-loaded NDC samples were found to catalyze both WOR and ORR under light illumination. The chemical pathways initiated by the pristine and metal-loaded NDC were investigated. This study provides valuable insights into potential mechanisms relevant to the early evolution of our planet.
With the impact of energy crisis and environmental problems, it is urgent to develop green sustainable energy. Osmotic energy stored in the salinity difference between seawater and river water is one of the sustainable, abundant, and renewable energy. However, the membranes used to capture osmotic energy by reverse electrodialysis (RED) always suffer from low ion selectivity, low stability and low power. Hydrogels with three-dimensional (3D) networks have shown great potential for ion transportation and energy conversion. In this work, based on the homogeneity and porosity characteristics of acrylamide (AM) hydrogel, as well as the remarkable stability and abundant negative charge of 3-sulfopropyl acrylate potassium salt (SPAK), a high-performance AM/SPAK cation-selective hydrogel membrane was successfully developed for harvesting osmotic energy. Compared to AM hydrogels, utilizing AM/SPAK as a monomer mixture greatly facilitated the preparation of homogeneous polymers, exhibiting a porous structure, exceptional ion selectivity, and remarkable stability. A maximum output power density of 13.73 W/m2 was achieved at a 50-fold NaCl concentration gradient, exceeding the commercial requirement of 5 W/m2. This work broadens the idea for the construction and application of composite hydrogel in high efficiency osmotic energy conversion.
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