Latest ArticlesRecently, non-centrosymmetric (NCS) Hg-based chalcogenides have garnered significant interest due to their strong second-harmonic-generation intensities (deff), making them attractive candidates for infrared nonlinear optical (IR-NLO) application. However, achieving both wide band gaps (Eg) and large phase-matched deff simultaneously in these materials remains a challenge due to their inherent constraints on each other. In this research, we have successfully obtained two quaternary NCS Hg-based chalcogenides, Rb2HgGe3S8 and Cs2HgGe3S8, by implementing a bandgap engineering strategy that involves alkali metal introduction and Hg/Ge ratio regulation. Both compounds consist of 2D [HgGe3S8]2– anionic layers made of 1D [HgGeS6]6– chains and dimeric [Ge2S6]4– polyhedra arranged alternately, and the charge-balanced Rb+/Cs+ cations located between these layers. Remarkably, Rb2HgGe3S8 and Cs2HgGe3S8 exhibit overall properties required for promising IR-NLO materials, including sufficient PM deff (0.55–0.70 × AgGaS2@2050 nm), large Eg (3.27–3.41 eV), giant laser-induced damage thresholds (17.4–19.7 × AgGaS2@1064 nm), broad optical transmission intervals (0.32–17.5 µm), and suitable theoretical birefringence (0.069–0.086@2050 nm). Furthermore, in-depth theoretical analysis reveals that the exceptional IR-NLO performance is attributed to the synergy effects of distorted [HgS4] and [GeS4] tetrahedra. Our study provides a useful strategy for enhancing the Eg and advancing Hg-based IR-NLO materials, which is expected to extended and implemented in other chalcogenide systems.
Post-synthetic installation strategy is an effective approach to improve the functions of metal-organic frameworks (MOFs). Herein, a pair of chiral MOFs is successfully constructed through solvothermal subcomponent self-assembly and exhibit circularly polarized luminescence (CPL). These MOFs contain coordinatively unsaturated Zn sites and channels, which allow the installation of pyridyl-terminated pillars into the original structure. Such a post-synthetic installation process reinforces the MOFs' rigidity and increases the photoluminescence quantum yields (PLQYs). Furthermore, the luminescence dissymmetry factors (glum) of these post-modified MOFs are amplified after installing the pillars. This work provides an appealing strategy for boosting the CPL performance of chiral MOFs.
Lithium argyrodites Li6PS5X (X = Cl, Br, I) show great potential as solid electrolytes for solid-state lithium batteries due to their high Li-ion conductivities and excellent electrode compatibility. However, the relatively low conductivity of Li6PS5I (10−6 mS/cm) compared to the other two compositions limits its applications. Herein, Si-doped Li6.5P0.5Si0.5S5I electrolyte is designed and synthesized with superior high conductivity of 3.6 mS/cm. Structural characterization proves the increase due to the anion disorder and volume expansion caused by Si-doping. However, the poor interfacial stability between layered oxide cathode LiNi0.6Co0.2Mn0.2O2 and Li6.5P0.5Si0.5S5I inhibits its battery performance. By introducing Li3InCl6 electrolyte in the configuration, the corresponding battery delivers high initial discharge capacity of 150.2 mAh/g and superior cyclability during 250 cycles at 0.5 C. This work offers design strategy to obtain Li6PS5I-based electrolytes for high performance solid-state batteries.
Aqueous alkaline zinc batteries (AZBs) exhibit great potential due to their high capacity, high safety and low cost. However, despite these advantages, the lack of high stability and high utilization rate makes the search for high-performance cathode materials a great challenge. Here, an amorphous nickel boride/rGO (NiB/rGO) complex structure was designed. As a result of abundant unsaturated active sites and synergistic electronic effects, amorphous NiB exhibits excellent energy storage properties. As well as having high electrical conductivity, rGO avoids aggregation of NiB nanoparticles, ensuring that NiB/rGO electrodes have a high energy storage capacity. The structure has a strong adhesion between NiB and rGO, which protects its stable structure and extends its life. More importantly, the NiB/rGO//Zn full battery shows remarkable capacity (228.4 mAh/g at 2 A/g), extraordinary cycle durability (93.7% retained after 1000 cycles) and strong energy density 399.7 Wh/kg, when coupled with NiB/rGO cathode. This work will also shed light on other nickel-zinc batteries in order to achieve super durability and capacity.
Magnesium rechargeable batteries (MRBs) present opportunities for grid-scale energy storage applications as a complement to Li-ion batteries (LIBS). The major challenges are the low reversible capacity, inferior cycling stability and unsatisfactory energy densities. Na3VCr0.5Fe0.5(PO4)3 with a well-defined NASION-type structure is used as cathode in Mg cell. Two-electrons reaction (~116 mAh/g), 1.5 V average voltage and 65% of capacity retention over 100 cycles are accomplished. Mg is inserted by a biphasic reaction with the participation of V3+/V4+/V5+ redox couples in the electrochemical reaction while the non-active redox couples such as Cr3+/Cr4+ and Fe2+/Fe3+ served as stabilizer to buffer the volume variation. A thermal stability up to ~412 ℃ is also exhibited. Therefore, incorporating a mixture of three transition metal (V/Cr/Fe) in this type of structures will broaden new perspectives for realizing high performance cathodes for MRBs.
Na-ion cathode materials with a fast charge and discharge behavior are needed to develop future high-energy sodium-ion batteries (SIBs). However, inevitably complicated phase transitions and sluggish kinetics during insertion and removal of Na+ in P2-type layered transition metal oxides generate structural instability and severe capacity decay. To get rid of such a dilemma, we report a structural optimization strategy to promote P2-type layered transition metal oxides with more (010) active planes as an efficient cathode for SIBs. As a result, as-prepared hexagonal-prism P2-type layered Na0.71Ni0.16Li0.09Co0.16Mn0.6O2 cathode with more (010) active planes delivers a reversible capacity of 120.1 mAh/g at 0.1 C, impressive rate capability of 52.7 mAh/g at 10 C, and long-term cycling stability (capacity retention of 95.6% over 200 cycles). The outstanding electrochemical performance benefited from the unique hexagonal-prism with more (010) active facets, which can effectively shorten the diffusion distances of Na+, increase the Na-ion migration dynamics and nanostructural stability during cycling verified by morphology characterization, Rietveld refinement, GITT, density functional theory calculations and operando XRD.
Metronidazole (MNZ) is a type of antibiotic that can help people and animals cure bacterial infections, however, abuse of MNZ has posed a threat to human health. Hence, portable and visual detection of MNZ is meaningful for food safety and rational administration of drugs, but full of challenges. Hence, a porous three-dimensional Tb-based metal-organic framework (MOF) {(CH3)2NH2·[Tb5(TDA)8(H2O)2]·6DMF·2C2H5OH}n (TDA-Tb) with good solvent and pH stabilities was prepared, and the framework possesses one-dimensional channels with a diameter of 12 Å along the c-axis. Experiment results suggest that the synthesized TDA-Tb can selectively and sensitively detect MNZ in water, and the limit of detection (LOD) is as low as 4.1 × 10−7 mol/L. Moreover, a flexible sensor TDA-Tb-M was also constructed by incorporating TDA-Tb into membrane materials for convenient usage. And the TDA-Tb-M firstly realized portable and visual detection of MNZ through smartphone scanning, which may inspire more probes with wide application ranges.
The combination of interface engineering and defect engineering is a promising strategy for developing new semiconducting surface-enhanced Raman scattering (SERS) substrate. Herein, an organic/inorganic hybrid g-C3N4/TiO2-X heterojunction with synchronous generation of strong interface effect and abundant surface oxygen vacancy (OV) defect was prepared by a simple sol-hydrothermal procedure with a help of urea. Due to the improved substrate-to-molecule charge transfer (CT) from joint contribution of high-efficiency carrier separation induced by strong interface coupling effect and multiple CT paths derived from abundant surface OV, g-C3N4/TiO2-X substrate exhibits greatly enhanced SERS effect for non-resonant 4-mercaptobenzoic acid (4-MBA) probe. The enhancement factor of g-C3N4/TiO2-X substrate for 4-MBA is as high as 5.57 × 106, and the substrate exhibits ultra-high stability and excellent spectral reproducibility. More meaningfully, the developed g-C3N4/TiO2-X heterojunction can be used to execute an ultrasensitive detection for antibiotic residues in real water system, even comprehensive evaluation of multi-component residues.
Water splitting with proton exchange membrane water electrolyzers (PEMWE) is regarded as a promising pathway for sustainable hydrogen conversion. Additionally, oxygen evolution reaction (OER) is considered as the dominant factor during the whole process due to the sluggish kinetics. Among the catalysts, Ru-based catalysts draw special attention because of their excellent activity and relatively low price. However, the limited stability impedes their further commercialization and tremendous efforts have been devoted to overcome this challenge. This review firstly introduces the basic mechanisms of OER. Then the evaluation protocols and techniques to investigate the stability of Ru-based catalysts are summarized. A detailed elucidation of the possible degradation mechanisms is also critically analyzed. Furthermore, effective strategies to design durable Ru-based catalysts for acidic OER are discussed. Such as heteroatom doping, phase and facet engineering, heterostructure building and support optimization. Finally, promises, perspectives and challenges in developing highly durable Ru-based catalysts for acidic OER are outlined.
For a significant duration, enhancing the efficacy of cancer therapy has remained a critical concern. Magnetotactic bacteria (MTB), often likened to micro-robots, hold substantial promise as a drug delivery system. MTB, classified as anaerobic, aquatic, and gram-negative microorganisms, exhibit remarkable motility and precise control over their internal biomineralization processes. This unique ability results in the formation of magnetic nanoparticles arranged along filamentous structures in a catenary fashion, enclosed within a membrane. These bacteria possess distinctive biochemical properties that facilitate their precise positioning within complex environments. By harnessing these biochemical attributes, MTB could potentially offer substantial advantages in the realm of cancer therapy. This article reviews the drug delivery capabilities of MTB in tumor treatment and explores various applications based on their inherent properties. The objective is to provide a comprehensive understanding of MTB-driven drug delivery and stimulate innovative insights in this field.
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