Latest ArticlesHerein, the Cu(Ⅲ) synthesized from copper plating effluent was developed for the first time to evaluate the onsite degradation performance of heavy metal complexes in the wastewater, thus achieving the purpose of "treating waste with waste". The results indicated that synthetic Cu(Ⅲ) presented the excellent decomplexation performance for Cu(Ⅱ)/Ni(Ⅱ)-organic complexes. The removal efficiency of Cu(Ⅱ)/Ni(Ⅱ)-EDTA significantly increased with increasing Cu(Ⅲ) dosage, and the degradation of Cu(Ⅱ)/Ni(Ⅱ)-EDTA by synthetic Cu(Ⅲ) system displayed highly pH-dependent reactivity. The radical quencher experiments confirmed that Cu(Ⅲ) direct oxidation were mainly involved in the degradation of Cu(Ⅱ)-EDTA. Additionally, the continuous decarboxylation process was proven to be the main degradation pathway of Cu(Ⅱ)-EDTA in Cu(Ⅲ) system. The coexisting substances (SO42−, Cl− and fulvic acids) showed little impacts at low level for the removal of Cu(Ⅱ)/Ni(Ⅱ)-EDTA, while retarded the degradation of Cu(Ⅱ)-EDTA slightly at high level, which features high selective oxidation. Encouragingly, it was also effective to remove Cu(Ⅱ)/Ni(Ⅱ)-EDTA from in treating actual Cu/Ni-containing wastewater through synthetic Cu(Ⅲ) treatment.
Improving the surface atoms utilization efficiency of catalysts is extremely important for large-scale H2 production by electrochemical water splitting, but it remains a great challenge. Herein, we reported two kinds of MoO3-polyoxometalate hybrid nanobelt superstructures (MoO3-POM HNSs, POM= PW12O40 and SiW12O40) using a simple hydrothermal method. Such superstructure with highly uniform nanoparticles as building blocks can expose more surface atoms and emanate increased specific surface area. The incorporated POMs generated abundant oxygen vacancies, improved the electronic mobility, and modulated the surface electronic structure of MoO3, allowing to optimize the H* adsorption/desorption and dehydrogenation kinetics of catalyst. Notably, the as-prepared MoO3-PW12O40 HNSs electrodes not only displayed the low overpotentials of 108 mV at 10 mA/cm2 current density in 0.5 mol/L H2SO4 electrolyte but also displayed excellent long-term stability. The hydrogen evolution reaction (HER) performance of MoO3-POM superstructures is significantly better than that of corresponding bulk materials MoO3@PW12O40 and MoO3@SiW12O40, and the overpotentials are about 8.3 and 4.9 times lower than that of single MoO3. This work opens an avenue for designing highly surface-exposed catalysts for electrocatalytic H2 production and other electrochemical applications.
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.
Herein, an alkyne-terminated acid/base responsive amphiphilic [2]rotaxane shuttle was synthesized, and then modified onto the glass surface through "click" reaction. The XPS N 1s spectrum and contact-angle measurement were performed to prove the successful immobilization. The amphiphilic [2]rotaxane functionalized surface presented controllable wettability responding to external acid-base stimuli. This bistable rotaxane modified material system promoted the practical application of molecular machines.
Excessive Fe3+ ion concentrations in wastewater pose a long-standing threat to human health. Achieving low-cost, high-efficiency quantification of Fe3+ ion concentration in unknown solutions can guide environmental management decisions and optimize water treatment processes. In this study, by leveraging the rapid, real-time detection capabilities of nanopores and the specific chemical binding affinity of tannic acid to Fe3+, a linear relationship between the ion current and Fe3+ ion concentration was established. Utilizing this linear relationship, quantification of Fe3+ ion concentration in unknown solutions was achieved. Furthermore, ethylenediaminetetraacetic acid disodium salt was employed to displace Fe3+ from the nanopores, allowing them to be restored to their initial conditions and reused for Fe3+ ion quantification. The reusable bioinspired nanopores remain functional over 330 days of storage. This recycling capability and the long-term stability of the nanopores contribute to a significant reduction in costs. This study provides a strategy for the quantification of unknown Fe3+ concentration using nanopores, with potential applications in environmental assessment, health monitoring, and so forth.
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.
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.
Birefringent crystals play an irreplaceable role in optical systems by adjusting the polarization state of light in optical devices. This work successfully synthesized a new thiophosphate phase of β-Pb3P2S8 through the high-temperature solid-state spontaneous crystallization method. Different from the cubic α-Pb3P2S8, the β-Pb3P2S8 crystallizes in the orthorhombic Pbcn space group. Notably, β-Pb3P2S8 shows a large band gap of 2.37 eV in lead-based chalcogenides, wide infrared transparent window (2.5−15 µm), and excellent thermal stability. Importantly, the experimental birefringence shows the largest value of 0.26@550 nm in chalcogenides, even larger than the commercialized oxide materials. The Barder charge analysis result indicates that the exceptional birefringence effect is mainly from the Pb2+ and S2− in the [PbSn] polyhedrons. Meanwhile, the parallelly arranged polyhedral layers could improve the structural anisotropic. Therefore, this work supports a new method for designing chalcogenides with exceptional birefringence effect in the infrared region.
Optimizing the interfacial quality of halide perovskites heterojunction to promote the photogenerated charge separation is of great significance in photocatalytic reactions. However, the delicately regulation of interfacial structure and properties of halide perovskites hybrid is still a big challenge owing to the growth uncontrollability and incompatibility between different constituents. Here we use BiOBr nanosheets as the start-template to in situ epitaxially grow Cs3Bi2Br9 nanosheets by “cosharing” Bi and Br atoms strategy for designing a 2D/2D Cs3Bi2Br9/BiOBr heterojunction. Systematic studies show that the epitaxial heterojunction can optimize the synergistic effect of BiOBr and Cs3Bi2Br9 via the formation of tight-contact interfaces, strong interfacial electronic coupling and charge redistribution, which can not only drive the Z-scheme charge transfer mechanism to greatly promote the spatial separation of electron-hole pairs, but also modulate the interfacial electronic structure to facilitate the adsorption and activation of toluene molecules. The heterojunction exhibited 62.3 and 2.4-fold photoactivity improvement for toluene oxidation to benzaldehyde than parental BiOBr and Cs3Bi2Br9, respectively. This study not only proposed a novel dual atom-bridge protocol to engineer high-quality perovskite heterojunctions, but also uncovered the potential of heterojunction in promoting electron-hole separation as well as the application in photocatalytic organic synthesis.
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