Water-splitting devices for hydrogen generation through electrolysis (hydrogen evolution reaction, HER) hold great promise for clean energy. However, their practical application relies on the development of inexpensive and efficient catalysts to replace precious platinum catalysts. We previously reported that HER can be largely enhanced through finely tuning the energy level of molybdenum sulfide (MoS) by hot electron injection from plasmonic gold nanoparticles. Under this inspiration, herein, we propose a strategy to improve the HER performance of MoS by engineering its energy level via direct transition-metal doping. We find that zinc-doped MoS (Zn-MoS) exhibits superior electrochemical activity toward HER as evidenced by the positively shifted onset potential to -0.13 V vs RHE. A turnover of 15.44 s at 300 mV overpotential is achieved, which by far exceeds the activity of MoS catalysts reported. The large enhancement can be attributed to the synergistic effect of electronic effect (energy level matching) and morphological effect (rich active sites) via thermodynamic and kinetic acceleration, respectively. This design opens up further opportunities for improving electrocatalysts by incorporating promoters, which broadens the understanding toward the optimization of electrocatalytic activity of these unique materials.
Direct photocatalysis making use of plasmonic metals has attracted significant attention due to the light-harnessing capabilities of these materials associated with localized surface plasmon resonance (LSPR) features. Thus far, most reported work has been limited to plasmon-induced chemical transformations. Herein, we demonstrate that electrochemical reactions can also be accelerated by plasmonic nanoparticles upon LSPR excitation. Using glucose electrocatalysis as a model reaction system, the direct plasmon-accelerated electrochemical reaction (PAER) on gold nanoparticles is observed. The wavelength- and solution-pH-dependent electrochemical oxidation rate and the dark-field scattering spectroscopy results confirm that the hot charge carriers generated during plasmon decay are responsible for the enhanced electrocatalysis performance. Based on the proposed PAER mechanism, a plasmon-improved glucose electrochemical sensor is constructed, demonstrating the enhanced performance of the non-enzyme sensor upon LSPR excitation. This plasmon-accelerated electrochemistry promises potential applications in (bio)electrochemical energy conversion, electroanalysis, and electrochemical devices.
As one of the common reactive oxygen species, H2O2 has been widely used for combating pathogenic bacterial infections. However, the high dosage of H2O2 can induce undesired damages to normal tissues and delay wound healing. In this regard, peroxidase‐like nanomaterials serve as promising nanozymes, thanks to their positive promotion toward the antibacterial performance of H2O2, while avoiding the toxicity caused by the high concentrations of H2O2. In this work, ultrasmall Au nanoparticles (UsAuNPs) are grown on ultrathin 2D metal–organic frameworks (MOFs) via in situ reduction. The formed UsAuNPs/MOFs hybrid features both the advantages of UsAuNPs and ultrathin 2D MOFs, displaying a remarkable peroxidase‐like activity toward H2O2 decomposition into toxic hydroxyl radicals (·OH). Results show that the as‐prepared UsAuNPs/MOFs nanozyme exhibits excellent antibacterial properties against both Gram‐negative (Escherichia coli) and Gram‐positive (Staphylococcus aureus) bacteria with the assistance of a low dosage of H2O2. Animal experiments indicate that this hybrid material can effectively facilitate wound healing with good biocompatibility. This study reveals the promising potential of a hybrid nanozyme for antibacterial therapy and holds great promise for future clinical applications.
The growth of atomically dispersed metal catalysts (ADMCs) remains a great challenge owing to the thermodynamically driven atom aggregation. Here we report a surface-limited electrodeposition technique that uses site-specific substrates for the rapid and room-temperature synthesis of ADMCs. We obtained ADMCs by the underpotential deposition of a non-noble single-atom metal onto the chalcogen atoms of transition metal dichalcogenides and subsequent galvanic displacement with a more-noble single-atom metal. The site-specific electrodeposition enables the formation of energetically favorable metal–support bonds, and then automatically terminates the sequential formation of metallic bonding. The self-terminating effect restricts the metal deposition to the atomic scale. The modulated ADMCs exhibit remarkable activity and stability in the hydrogen evolution reaction compared to state-of-the-art single-atom electrocatalysts. We demonstrate that this methodology could be extended to the synthesis of a variety of ADMCs (Pt, Pd, Rh, Cu, Pb, Bi, and Sn), showing its general scope for functional ADMCs manufacturing in heterogeneous catalysis.
BackgroundAstrocytomas are the most common and aggressive brain tumors characterized by their highly invasive growth. Gain of chromosome 7 with a hot spot at 7q32 appears to be the most prominent aberration in astrocytoma. Previously reports have shown that microRNA-335 (miR-335) resided on chromosome 7q32 is deregulated in many cancers; however, the biological function of miR-335 in astrocytoma has yet to be elucidated.ResultsWe report that miR-335 acts as a tumor promoter in conferring tumorigenic features such as growth and invasion on malignant astrocytoma. The miR-335 level is highly elevated in C6 astrocytoma cells and human malignant astrocytomas. Ectopic expression of miR-335 in C6 cells dramatically enhances cell viability, colony-forming ability and invasiveness. Conversely, delivery of antagonist specific for miR-335 (antagomir-335) to C6 cells results in growth arrest, cell apoptosis, invasion repression and marked regression of astrocytoma xenografts. Further investigation reveals that miR-335 targets disheveled-associated activator of morphogenesis 1(Daam1) at posttranscriptional level. Moreover, silencing of endogenous Daam1 (siDaam1) could mimic the oncogenic effects of miR-335 and reverse the growth arrest, proapoptotic and invasion repression effects induced by antagomir-335. Notably, the oncogenic effects of miR-335 and siDAAM1 together with anti-tumor effects of antagomir-335 are also confirmed in human astrocytoma U87-MG cells.ConclusionThese findings suggest an oncogenic role of miR-335 and shed new lights on the therapy of malignant astrocytomas by targeting miR-335.
Sodium
iron phosphate (Na3Fe2(PO4)3) as cathode material for sodium-ion batteries has been
synthesized through a simple method of a solid state reaction. It
crystallizes in a monoclinic structure in the space group C2/c. The morphology of the as-prepared
sample has been investigated by scanning electron microscopy and transmission
electron microscopy. The charge/discharge curves show a very flat
plateau at about 2.5 V (vs Na/Na+). The initial specific
discharge capacity is 61 mAh g–1 and remains at
57 mAh g–1 after 500 cycles at a current rate of
1 C. X-ray photoelectron spectroscopy measurements indicate that not
all of the Fe3+ of Na3Fe2(PO4)3 is reduced during the electrochemical process.
The ex-situ X-ray diffraction measurements were applied
to research the mechanism of sodium-ion storage; the results indicated
that the Na3Fe2(PO4)3 compound
partly transformed into Na4Fe2(PO4)3 and Na3+x
Fe2(PO4)3 compound. These results testify to the
potential of monoclinic Na3Fe2(PO4)3 as a cathode material in sodium-ion batteries.
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