Here, a series of nitrogen-doped carbon (NC) supported transition metal oxide catalysts were prepared by pyrolysis of chitosan-metal salt mixtures for the efficient synthesis 2,5-diformylfuran (DFF) from 5-hydroxymethylfurfural (HMF) and fructose. Among them, supported molybdenum-based species on nitrogen-doped carbon (Mo/NC) exhibited excellent activity and selectivity for selective oxidation of HMF to DFF. The presence of nitrogen species reduces the electron cloud density around the Mo species, thereby improving the catalytic activity. Moreover, the interaction between active MoO2 species on the catalyst surface and NC ensured the stability of the catalyst, resulting in no significant loss of activity after four catalytic cycles. 99.5 % and 55.1 % yields of DFF with full conversion were obtained from HMF and fructose respectively over Mo/NC-chitosan-600 in DMSO under ambient air. In order to enhance DFF yield from fructose, sulfonate groups were introduced into Mo/NC-chitosan-600 catalyst, leading to the highest DFF yield of 70.2 %. In addition, this catalyst also allowed 10.0%, 22.9% and 33.3% DFF yields from glucose, sucrose and inulin, respectively.
Due to the complexity and diversity of infectious diseases, diagnosis based solely on symptoms and imaging manifestations is associated with a high rate of misdiagnosis, so it is particularly important to find reliable and accurate biomarkers. Four inflammatory biomarkers (CRP, IL-6, PCT and SAA) have different manifestations and roles in different infectious diseases and stages of infection, and the diagnosis and identification of infectious diseases can be realized through quantitative analysis of these four biomarkers simultaneously. In this study, we developed a colloidal gold nanoparticle (AuNP)-based multiplex LFA strip using eight highly-sensitive monoclonal antibodies that simultaneously detected CRP, IL-6, PCT and SAA in serum within 15 min. And quantitative analysis was achieved with a portable strip reader, the LODs were 2.5 μg/mL, 25.3 pg/mL 0.87 ng/mL and 8.8 μg/mL for CRP, IL-6, PCT and SAA, while detection ranges were 2.5–200 μg/mL, 25.3–8000 pg/mL 0.87–100 ng/mL and 8.8–200 μg/mL. Moreover, the quantitative colloidal gold assay correlated well with the results of a chemiluminescence immunoassay when testing clinical serum samples. Our developed method was reliable and accurate according to the recovery test results. Therefore, the strip can be used as an alternative method for the simultaneous monitoring of CRP, IL-6, PCT and SAA in serum samples.
Metal chelation, characterized by its precise interactions with diverse functional groups, assumes a pivotal role in providing structural stability and generating reactive centers within metalloproteins and metallopeptides. This, in turn, orchestrates the architecture and functionality of various biological processes in living organisms. In our biomimetic approach inspired by the intricacies of natural metallopeptides, we have purposefully designed pyridine-bis-tyrosine, a concise Metallopeptide Conjugate (sMPC). Demonstrating the capacity to form complexes with various bioactive metal ions, sMPC emerges as a promising tool for advancing our understanding of metal-binding proteins and catalyzing the development of cutting-edge biotechnological materials and technologies. Our investigations underscore the hierarchical self-assembly of these abridged conjugates into toroidal to vesicle nanostructures, influenced by concentration, and their susceptibility to spatial manipulation through metal ion coordination with functional groups. These biocompatible metal peptide complexes and their resultant nanomaterials present specific potential as exceptional therapeutic agents to address problems associated with metal ion deficiencies, offering a facile and low-cost alternative to traditional metallodrugs.
Electrochemical hydrogen and acetate cogeneration from ethanol is a promising green hydrogen production technique with low hydrogen production energy consumption and high profitability. However, the poor catalytic stability of the anodic ethanol electro-oxidation reaction (EOR) retards the device application. We adopted a metal support interaction strategy to reinforce small-sized Au active sites using cuprous sulfide supports. The Au−Cu2–xS/C showed a superior activity of 1055 mA mgAu−1 at 1.1 V vs. RHE and retained the high activity in the chronopotentiometric test, surpassing the Au/C catalyst. It was demonstrated that the Cu2–xS support facilitated the formation of Au−OH and prevented the gold sites from aggregation, leading to high activity and stability for EOR. Finally, an electrochemical cogeneration electrolyzer assembled with the Au−Cu2–xS/C anodic catalyst continuously ran for over 100 hours, suggesting the device‘s applicability.
Silver selenide (Ag2Se) is a promising thermoelectric material for near-room temperature applications. This study proposes a fast, simple, and cost-effective method for producing high thermoelectric performance bulk Ag2Se. Ag2Se powders were synthesized from Ag and Se powders via a one-hour wet ball milling process, followed by the fabrication of bulk pellets through low-temperature hot-pressing (130–250 °C) with a mere 0.5-hour holding time. Both Ag2Se powders and bulk pellets exhibited a single phase of Ag2Se with an orthorhombic structure. Moreover, uniform compositional distribution with the stoichiometric Ag : Se ratio was observed in all samples. Microstructural analysis revealed distinct grain boundaries in samples hot-pressed below 190 °C, transitioning to grain coalescence was at 190 °C and 250 °C. The thermoelectric and transport measurements demonstrated that the electrical conductivity decreased and the Seebeck coefficient increased with hot-pressing temperatures from 130 °C and 190 °C primarily due to reduced carrier concentrations. Thermal conductivity decreased with increasing hot-pressing temperatures up to 190 °C, attributed to the weak chemical bonding of Ag2Se and the presence of defects. This combination resulted in a peak zT over 1.0 at 300 K, with an average zT close to 1.0 from 300 to 380 K. In comparison to other reported synthesis methods, the present approach offers significantly reduced processing time, simplicity, and cost-effectiveness. Despite lower temperatures and shorter processing times, the method produces Ag2Se with zT values comparable to more intricate techniques. This fabrication route holds the potential for scalable mass production in the future.
With the growing demand for high-performance smart windows, the discover of a class of thermochromic materials with reversible cycling and rapid response characteristics has become urgent. In this work, we have uncovered a two-dimensional (2D) Ruddlesden-Popper (RP) phase halide perovskite, (PMA)2MAPb2I7−xClx, where PMA=C6H5CH2NH3 and MA=CH3NH3, exhibiting exceptional reversible thermochromic properties. The 2D RP phase perovskite thin film features a low transition temperature (Tc=30 °C from the hydrated state to the hot state, along with a fast transition time of 40 s. Furthermore, the addition of 0.5 times excess MAI significantly enhances the visible light transmittance of the hydrated state. Characteristic hydration peaks in X-ray diffraction patterns and O−H bond absorption peaks Fourier-transform infrared spectra are observed in the thin film in its hydrated state, which disappear in the hot state, validating its reversible thermochromic properties. Additionally, a solar cell based on the thermochromic 2D RP phase thin film achieves a power conversion efficiency of 2.31 %, offering a promising solution for advanced smart window technologies.
Calcium ions (Ca2+) are essential for a myriad of physiological functions, including excitability, neurotransmitter release, gene transcription, cell proliferation, synaptic plasticity, and hormone secretion. Consequently, the detection of Ca2+ concentrations in water is of fundamental and practical significance. In this study, a novel method for the simple, visual, and rapid colorimetric detection of Ca2+ is introduced, leveraging the surface plasmon resonance (SPR) absorbances of gold nanoparticles (AuNPs) modified with 5-Pyrimidinylboronic acid (5-PBA). A color change from wine-red to gray-blue was observed with increasing concentrations of Ca2+, indicative of the agglomeration of AuNPs. This agglomeration displayed favorable anti-interference properties and selectivity. The limits of detection (LOD) were determined to be 0.08 mM by the unaided eye and 3.29 μM by UV-visible spectroscopy. Moreover, an excellent linear relationship (R2=0.9879) was maintained within the Ca2+ concentration range of 0.0 to 0.5 mM. These results suggest that AuNPs modified with 5-PBA are suitable for the quantitative determination of Ca2+. Subsequent testing on actual samples confirmed that this new method could be effectively applied to the monitoring of Ca2+ in water.
Lead halide perovskites have been explored ardently in the past decade owing to their excellent photophysical properties. High-temperature cation exchange reactions have been employed to improve the stability and performance in perovskite lattice, but lacks control over size, shape, and stoichiometry. Herein, the solution phase interaction of cesium lead bromide (CsPbBr3) nanocrystals with monovalent and bivalent copper ions, under ambient conditions is systematically investigated. The introduction of Cu1+ explicitly initiates a one-dimensional growth with a distinct phase transition, that is from cubic to orthorhombic, while Cu2+ induces a partial exchange with Pb2+ with no phase change. DFT calculations suggest that Cu1+ induces structural distortion via Cs1+ substitution, altering the Goldschmidt tolerance factor and perovskite octahedral tilting, leading to the phase transition. Additionally, the oleic acid/amine ligands used to stabilize the nanocrystals, are preferentially etched away to form complexes with Cu1+, initializing an oriented growth of the nanocubes to nanorods. A mechanistic investigation of the evolution of the nanorods gave insights on tuning the tolerance factor via room temperature modifications and cation exchanges in perovskites for anisotropy and morphology tuning. This effortlessly obtained perovskite nanorods with Cu1+ could find effective applications in optoelectronics, and as novel photocatalysts.
Plasmonic transition metal nitrides (TMNs) have emerged as a low-cost and thermally and chemically robust alternatives to noble metals. While their superior thermal properties have been established, their chemical properties on the nanoscale haven't been as well investigated. Herein, the oxidative stability over time under ambient conditions and colloidal stability as function of pH was explored for plasmonic TiN, ZrN, and HfN nanoparticles. It was discovered that the TMN nanoparticles made via solid-state method had a narrow pH stability range between 2–3. Under highly acidic conditions, the particles underwent dissolution and at pH ≥4, they aggregate and precipitate from the solution. Additionally, TiN nanoparticles had poor oxidative stability and oxidized to TiO2 after ~40 days. 3-Aminopropyltriethoxysilane (APTES) and dimethylsilane coated TMNs were synthesized to yield water and organic solvent dispersible particles, respectively. These functionalized colloidal suspensions showed enhanced oxidative stability over 60 days and the APTES coating widened the pH stability window of TMNs to include physiological pH. This study shows that surface functionalization using M−O−Si linkages (where M=Ti, Zr, or Hf) can greatly enhance the stability, dispersibility and therefore applicability of plasmonic TMN nanoparticles.