Latest ArticlesSilicon based (Si-based) materials are considered to be the most promising anode materials for lithium-ion batteries (LIBs) due to their high specific capacity. However, the issues of poor electrical conductivity and volume expansion during cycling have not been effectively addressed. The optimum remedy is to select specific materials to establish an exceptional conductive and volume buffer structure to assist the Si materials to develop its excellent lithium storage properties. Here, Si particles were encapsulated into porous carbon fibers containing ultrafine Co particles (CP) to obtained Si-x@CP-y film. Among them, the addition of Si particles and the void structure was precisely regulated to achieve a superior electrode with a high specific capacity. Subsequently, the two-dimensional conductive material reduced graphene oxide (rGO) nanosheets were further incorporated to obtain Si-2@CP-2@rGO films with core@multi-shell structure. The final electrode was equipped with one-, two-, and three-dimensional electronic pathways to allow rapid electron transport, and featured with multi-layer buffer structure and reserved pores that could effectively mitigate volume changes. As expected, the free-standing Si-2@CP-2@rGO electrode delivered a high specific capacity of 1221.2 mAh/g after 100 cycles at 0.1 A/g in a half cell, and the assembled full cell showed 249.0 mAh/g after 200 cycles at 0.2 A/g, which fulfilled the lightweight requirement for new energy storage devices.
Surface chemistry focuses on the investigation of the adsorption, migration, assembly, activation, reaction, and desorption of atoms and molecules at surfaces. Surface chemistry plays the pivotal roles in both fundamental science and applied technology. This review will summarize the recent progresses on surface assembly, synthesis and catalysis investigated mainly by scanning tunneling microscopy and atomic force microscopy. Surface assemblies of water and small biomolecules, construction of Sierpiński triangles and surface chirality are summarized. On-surface synthesis of conjugated carbo- and heterocycles and other kinds of carbon nanostructures are surveyed. Surface model catalysis, including single-atom catalysis and electrochemical catalysis, are discussed at the single-atom level.
Diabetic pressure ulcers (DPU) are non-healing due to vascular dysfunction and bacterial infection. Early intervention can delay ulcer progression, such as preventing the formation of full-thickness skin defects. Local administration of deferoxamine (DFO) at wound sites has been shown to promote neovascularization and enhance wound healing. However, since DPU skin wounds are not full-thickness defects and DFO is hydrophilic, enhancing its transdermal delivery is crucial for effective treatment. Photothermal ablation of stratum corneum, generated by copper sulfide nanoparticles (CuS NPs) under near-infrared (NIR) light irradiation, is a promising method to improve transdermal drug delivery. Meanwhile, CuS NPs-induced photothermal therapy offers excellent antibacterial performance. In this study, DFO and CuS NPs were incorporated into a matrix metalloproteinase (MMPs)-sensitive hydrogel. This hydrogel promotes cell adhesion and is degraded by cell-secreted MMPs, a process crucial for the controlled release of encapsulated DFO and CuS NPs. Under NIR irradiation, the stratum corneum is disrupted, facilitating transdermal DFO delivery and simultaneously eliminating infected bacteria. As a result, the essential requirements for DPU treatment, "facilitating transdermal DFO delivery, promoting angiogenesis, and inhibiting bacterial infection", were achieved simultaneously.
Since the discovery of the Nernst effect in 19th century, it has been an important transverse thermoelectric charge transport phenomenon in solid states. Conjugated polymers have recently attracted great attention as promising optoelectronic materials. However, the Nernst effect is yet to be explored for conducting polymers. Here, we report the first theoretical investigations of the Nernst effect in doped conducting polymers by first-principles calculations under the frame work of Fermi-liquid theory. Specifically, the Nernst coefficients of PBTTT are found to be ranging from 0.0029 to 0.039 µV K−1 T−1. They are monotonically decreased with the doping level due to both much enhanced Fermi energy and the decreased charge mobility at high doping level. Our theoretical findings not only enhance our fundamental understanding of the doping mechanism that controls the charge transport properties of conducting polymers, but more importantly, they also offer initial predictions of the transverse thermoelectric conversion capability of conducting polymers. These predictions are crucial for the development of future flexible thermoelectric applications based on the Nernst effect.
Matrix-assisted laser desorption ionization-mass spectrometry imaging (MALDI-MSI) has shown its capability in visualizing the spatial distribution of various kinds of endogenous metabolites. Nevertheless, high quality mass imaging of low polar metabolites remains challenging. Herein, a platform for sensitive matrix-assisted laser desorption ionization-mass spectrometry imaging of cholesterol and glycerides has been proposed. In the platform, a vacuum promoted on-tissue derivatization strategy was proposed to constantly make the derivatization reaction proceed towards to the direction of products. Compared with traditional on-tissue derivatization procedure, the strategy improved the acquired intensity of derivatized glycerides about 50%. Additionally, the mass spectrometry image reflecting the signal ratio between 3 classes of glycerides was achieved to exploit the metabolic level of glycerides on tissue slice. Finally, the platform was applied to brain slices of Alzheimer's transgenic mice, type 2 diabetes mice and normal mice. Significant difference was found in mass spectrometry images reflecting the signal ratio of multiple endogenous metabolites. The work constructed a promising platform for mapping of glycerides in tissue by mass spectrometry imaging.
The rational design of high-performance bifunctional electrocatalysts for overall water splitting (OWS) is the key to popularize hydrogen production technology. The active metal oxyhydroxide (MOOH) formed after surface self-reconfiguration of transition metal sulfide (TMS) electrocatalyst is often regarded as the "actual catalyst" in oxygen evolution reaction (OER). Herein, an Fe doped CoS2/MoS2 hollow TMS polyhedron (Fe-CoS2/MoS2) with rich Mott-Schottky heterojunction is reported and directly utilized as an OWS electrocatalyst. The spontaneous built-in electric field (BEF) at the heterogeneous interface regulates the electronic structure and D-band center of the catalyst. More importantly, the “TMS-MOOH” core-shell structure obtained in the KOH electrolyte shows enhanced OER properties. And the introduction of Fe ions activates the inert basal plane of MoS2, which greatly steps up the performance of HER. Hence, the preferable Fe-CoS2/MoS2–400 presents superior OER activity (η10 = 178 mV, η100 = 375 mV), HER activity (η10 = 92 mV) and ultra-high stability for 50 h. This work has deeply explored the catalytic mechanism of TMS and provided a new idea for the construction of efficient bifunctional catalysts.
Herein, a diatomite biomorphic Si-O doped carbon-based catalyst (DB-SiOC) was prepared using natural mineral diatomite as the silicon source and porous template. The results showed that the metal-free DB-SiOC catalyst exhibited ultrafast oxidation towards chlorophenol (CP) via peroxymonosulfate (PMS) activation, which was almost one order of magnitudes than most of carbon-based catalysts. The DB-SiOC/PMS system also showed the high ability to resist the interference of environmental matrix. The radicals (•OH and SO4•‒) exhibited a very small contribution to the CP oxidation while the electron transfer processes (ETP) played the major role in the DB-SiOC/PMS system. The electron shuttles from the electron-donating CP molecules to the adjacent DB-SiOC/PMS* could be efficiently triggered via Si-O bonds as bridges, making it possible for ultrafast oxidation of CP. In addition, the hollow-disc shaped DB-SiOC provided the biomorphic DE structures with abundant pores for enriching the PMS and pollutants, thus further accelerating the oxidation reaction. This work provided a new routine for the fabrication of Si-O doped carbon-based catalysts with excellent Fenton-like catalytic activity, which would greatly promote their application prospects in Fenton-like systems.
Two o-carborane based tetraphenylethene (TPE) cationic cyclophanes O1·4PF6 and O2·4PF6 were synthesized through an SN2 reaction. Their structures were confirmed both possessing Z-shaped cavities in single crystal analysis. The optical properties of these macrocycles were systematically investigated using UV–vis spectroscopy and fluorescence techniques. It is worth noting that the introduction of a methoxy group to the TPE unit enables the synthesis of a near-infrared-emitting macrocycle O2·4PF6. The recognition behaviors of these two macrocycles towards nucleotides were investigated using various techniques including fluorescence titration, UV–vis titration, and transmission electron microscopy (TEM). Interestingly, these cyclophanes exhibited aggregation-induced emission (AIE) effects in water or under the induction of nucleotides.
Selenium (Se) plays an important role in the development and treatment of lung cancer, yet its specific mechanisms remain elusive. Lower Se level in serum was noted in lung cancer patients compared to normal controls. Therefore, developing effective therapeutic adjuvants containing Se might benefit the treatment of lung cancer patients. This study aimed to investigate the association between Se and the chemotherapeutic efficacy of lung cancer. Lentinan-modified selenium nanoparticles (LET-SeNPs) were created to develop and verify the effectiveness of Se containing adjuvant applied with pemetrexed on lung cancer cells. A synergistic effect was observed between LET-SeNPs and pemetrexed in vitro. The combination of LET-SeNPs and pemetrexed could induce reactive oxygen species overproduction, mitochondrial dysfunction and DNA damage, ultimately leading to cancer cell apoptosis. It is implied that LET-SeNPs might be a promising sensitizer to pemetrexed chemotherapy and could potentially enhance chemotherapy efficiency in non-small cell lung cancer.
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