Latest ArticlesThe abuse of antibiotics has brought great harm to the human living environment and health, so it is extremely significant to develop an efficient and simple method to detect trace antibiotic residues in various wastewaters. Herein, a new two-dimensional (2D) Cd-based metal−organic framework (Cd-MOF, namely LCU-111) and its mixed matrix membranes (MMMs) is sifted as luminescence sensors for efficient monitoring antibiotic nitrofurazone (NFZ) in various aqueous systems and applied as visible fingerprint identifying. The LCU-111 has good selectivity, sensibility, reproducibility and anti-interference for luminescent quenching NFZ with low detection limits (LODs) of 0.4567, 0.3649 and 0.8071 ppm in aqueous solution, HEPES biological buffer, and real urban Tuhai River water, respectively. Interestingly, the luminescent test papers and MMMs allow the NFZ sensing easier and more rapid by naked eyes, only with a low LOD of 0.8117 ppm for MMMs sensor. Notably, by combining multiple experiments with density functional theory (DFT) calculations, the photo-induced electron transfer (PET) quenching mechanism is further elucidated. More importantly, potential practical applications of LCU-111 for latent fingerprint visualization provide lifelike evidences for effective identification of individuals, which can be applied in criminal investigation.
Li2ZrCl6 (LZC) solid-state electrolytes (SSEs) have been recognized as a candidate halide SSEs for all-solid-state Li batteries (ASSLBs) with high energy density and safety due to its great compatibility with 4 V-class cathodes and low bill-of-material (BOM) cost. However, despite the benefits, the poor chemical/electrochemical stability of LZC against Li metal causes the deterioration of Li/LZC interface, which has a detrimental inhibition on Li+ transport in ASSLBs. Herein, we report a composite SSE combining by LZC and argyrodite buffer layer (Li6PS5Cl, LPSC) that prevent the unfavorable interaction between LZC and Li metal. The Li/LPSC-LZC-LPSC/Li symmetric cell stably cycles for over 1000 h at 0.3 mA/cm2 (0.15 mAh/cm2) and has a high critical current density (CCD) value of 2.1 mA/cm2 at 25 ℃. Under high temperature (60 ℃) which promotes the reaction between Li and LZC, symmetric cell fabricated with composite SSE also display stable cycling performance over 1200 h at 0.3 mAh/cm2. Especially, the Li/NCM ASSLBs fabricated with composite SSE exhibit a high initial coulombic efficiency, as well as superior cycling and rate performance. This simple and efficient strategy will be instrumental in the development of halide-based high-performance ASSLBs.
Kirsten rat sarcoma viral oncogene homolog (KRAS)–phosphodiesterase-delta (PDEδ) is a promising target for antitumor drug discovery. Herein, highly efficient and environmentally sensitive fluorescent probes of PDEδ (DS-Probes) were rationally designed. As compared with the reported PDEδ probes, DS-Probes showed higher binding affinity and selectivity, which were able to conveniently and efficiently label PDEδ in live cells as well as tumor tissues. Therefore, these fluorescent probes are expected to facilitate PDEδ-based mechanism elucidation, drug discovery and pathologic diagnosis.
To address the insulating nature and the shuttle effect of iodide species that would deteriorate the battery performance, herein iron nitride is well-dispersed into porous carbon fibers with good flexibility via the facile electrospinning method and subsequent pyrolysis. The polyacrylonitrile precursor introduces the nitrogen doping under thermal treatment while the addition of iron acetylacetonate leads to the in-situ formation of iron nitride among the carbon matrix. The crucial pyrolysis procedure is adjustable to determine the hierarchical porous structure and final composition of the novel carbon fiber composites. As the self-supporting electrode for loading iodine, the zinc-iodine battery exhibits a large specific capacity of 214 mAh/g and good cycling stability over 1600 h. In the combination of in-situ/ex-situ experimental measurements with the theoretical analysis, the in-depth understanding of intrinsic interaction between composited support and iodine species elucidates the essential mechanism to promote the redox kinetics of iodine via the anchoring effect and electrocatalytic conversion, thus improving cycling life and rate performance. Such fundamental principles on the basic redox conversion of iodine species would evoke the rational design of advanced iodine-based electrodes for improving battery performance.
The solid electrolyte interphase (SEI), a passivation film covering the electrode surface, is crucial to the lifetime and efficiency of the lithium-ion (Li-ion) battery. Understanding the Li-ion diffusion mechanism within possible components in the mosaic-structured SEI is an essential step to improve the Li-ion conductivity and thus the battery performance. Here, we investigate the Li-ion diffusion mechanism within three amorphous SEI components (i.e., the inorganic inner layer, organic outer layer, and their mixture with 1:1 molar ratio) via ab initio molecular dynamic (AIMD) simulations. Our simulations show that the Li-ion diffusion coefficient in the inorganic layer is two orders of magnitude faster than that in the organic layer. Therefore, the inorganic layer makes a major contribution to the Li-ion diffusion. Furthermore, we find that the Li-ion diffusivity in the organic layer decreases slightly with the increase of the carbon chain from the methyl to ethyl owing to the steric hindrance induced by large groups. Overall, our current work unravels the Li-ion diffusion mechanism, and provides an atomic-scale insight for the understanding of the Li-ion transport in the SEI components.
Spectroscopic study of water splitting by neutral metal clusters is crucial to understanding the microscopic mechanism of catalytic processes but has been proven to be a challenging experimental target due to the difficulty in size selection. Here, we report a size-specific infrared spectroscopic study of the reactions between neutral group 3 metals and water molecules based on threshold photoionization using a vacuum ultraviolet laser. Quantum chemical calculations were carried out to identify the structures and to assign the experimental spectra. All the M2O4H4 (M = Sc, Y, La) products are found to have the intriguing M2(μ2-O)(μ2-H)(μ2-OH)(η1-OH)2 structures, indicating that the HOH bond breaking, the MO/MH/MOH bond formation, and hydrogen production proceed efficiently in the reactions between laser-vaporized metals and water molecules. The joint experimental and theoretical results on the atomic scale demonstrate that the water splitting by neutral group 3 metals is both thermodynamically exothermic and kinetically facile in the gas phase. These findings have important implications for unravelling the structure-reactivity relationship of catalysts with isolated metal atoms/clusters dispersed on supports.
Li-ion batteries with solid polymer electrolytes (SPEs) are safer than conventional liquid electrolytes due to the absence of highly flammable liquid electrolytes. However, their performance is limited by the poor Li+ transport in SPEs at room temperature. Anion-containing polymer-chains incorporated SPEs (ASPEs) are therefore developed to enhance Li+ diffusion kinetics. Herein, we propose a novel and feasible strategy to incorporate the anion-containing polymer-chains, such as lithiated perfluorinated sulfonic acid (PFSA), into polyvinylidene fluoride (PVDF) polymer-based SPEs. The immobile anion groups from the PFSA-chains impede the migration of mobile anion groups dissociated from the Li salt. The transference number is thus raised from ~0.3 to 0.52 with the introduction of anion-containing polymer-chains into SPEs. The electrostatic repulsion among anion-containing chains also reduces the close chain stacking and brings 159% increase in the ionic conductivity to 0.83 × 10−3 S/cm at 30 ℃ in contrast with the pure PVDF-based SPE. In addition, LiFeO4/Li batteries with ASPEs exhibit 55% capacity boost at 0.5 C in contrast to the capacity of batteries with pure-PVDF SPEs, and also offer more than 1000 charge/discharge cycles. Our research findings potentially offer a facile strategy to design thermal stable SPEs with superior Li+ transport behaviors towards developing high-performance SPEs-based batteries.
Lithium-halogen batteries (LHBs), including lithium iodide (Li-I2) and lithium bromide (Li-Br2) batteries, are receiving more attention for offering high energy density and excellent kinetic performance. However, LHBs commercialization is seriously hindered by the high solubility of halides, causing lower capacity and poor cyclability. This research covers the fabrication of a highly stable cathode of amorphous carbon coated CMK-3/LiI/LiBr nanocomposite for metal lithium batteries. The nanopores and coated layer can physically trap the dissolution of active materials. The amorphous carbon generated from polyacrylonitrile carries abundant nitrogen heteroatoms for the stable anchorage of halogens and halides via strong chemical adsorption. In addition, iodine can act as a complexing agent with bromine to reduce solvation energy. Consequently, the as-prepared CMK-3/LiI/LiBr/carbon (CIBP) nanocomposite cathode demonstrates an ultra-high reversible capacity of 407.4 mAh/g at the current density of 1.0 C performing up to 300 stable cycles.
Peptide and protein drugs with therapeutic effects suffer from their short half-life and low stability, albeit their high efficiency and specificity. To overcome these demerits, long-acting drug delivery systems have been developed, wherein poly(lactic-co-glycolic acid) (PLGA) implants are most preferred owing to their excellent biodegradability and biocompatibility. Dozens of PLGA based products have been approved since 1986, when the first product, named Decapeptyl®, successfully marched into market. To meet the increasing demand for delivering various peptides and proteins, different kinds of technologies have been developed for lab-scale fabrication or industrial manufacture. This review aims to introduce recent advances of PLGA implants, and give a brief summary of fundamental properties of PLGA, fabrication technologies of peptides/proteins-loaded PLGA implants as well as factors influencing the drug release processes. Moreover, challenges and future perspectives are also highlighted.
The sluggish conversion kinetics and shuttle effect of lithium polysulfides (LiPSs) severely hamper the commercialization of lithium–sulfur batteries. Numerous electrocatalysts have been used to address these issues, amongst which, transition metal dichalcogenides have shown excellent catalytic performance in the study of lithium–sulfur batteries. Note that dichalcogenides in different phases have different catalytic properties, and such catalytic materials in different phases have a prominent impact on the performance of lithium–sulfur batteries. Herein, 1T-phase rich MoSe2 (T-MoSe2) nanosheets are synthesized and used to catalyze the conversion of LiPSs. Compared with the 2H-phase rich MoSe2 (H-MoSe2) nanosheets, the T-MoSe2 nanosheets significantly accelerate the liquid phase transformation of LiPSs and the nucleation process of Li2S. In-situ Raman and X-ray photoelectron spectroscopy (XPS) find that T-MoSe2 effectively captures LiPSs through the formation of Mo-S and Li-Se bonds, and simultaneously achieves fast catalytic conversion of LiPSs. The lithium–sulfur batteries with T-MoSe2 functionalized separators display a fantastic rate performance of 770.1 mAh/g at 3 C and wonderful cycling stability, with a capacity decay rate as low as 0.065% during 400 cycles at 1 C. This work offers a novel perspective for the rational design of selenide electrocatalysts in lithium–sulfur chemistry.
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