Commercial nitric acid (HNO3) and ammonia (NH3) are mostly produced through the Ostwald process and the Haber-Bosch process, respectively. However, high energy demand and enormous greenhouse gas accompy these processes. The development of economical and green ways to synthesize HNO3 and NH3 is highly desirable for solving the global energy and environmental crisis. Here, we present two energy-efficient and environmentally friendly strategies to synthesize HNO3 and NH3 at distributed sources, including the electrocatalytic oxidation of N2 in air to HNO3 and the electrocatalytic reduction of residual ${\rm NO_{3}^{-}}$ contamination in water to NH3. The isotope-labeling studies combined with theoretical calculation reveal the reaction path of the two proposed strategies, confirming the origin of the electrochemical products. Importantly, the electrooxidation-generated ${\rm NO_{3}^{-}}$ ions may also serve as reactants for the electroreduction synthesis of NH3 in the future. Our work may open avenues for energy-efficient and green production of HNO3 and NH3 at distributed sources.
Hydantoin (imidazolidinedione) derivatives such as nitrofurantoin are small molecules that have aroused considerable interest recently due to their low rate of bacterial resistance. However, their moderate antimicrobial activity may hamper their application combating antibiotic resistance in the long run. Herein, we report the design of bacterial membrane-active hydantoin derivatives, from which we identified compounds that show much more potent antimicrobial activity than nitrofurantoin against a panel of clinically relevant Gram-positive and Gram-negative bacterial strains. These compounds are able to act on bacterial membranes, analogous to natural host-defense peptides. Additionally, these hydantoin compounds not only kill bacterial pathogens rapidly but also prevent the development of methicillin-resistant Staphylococcus aureus (MRSA) bacterial resistance under the tested conditions. More intriguingly, the lead compound exhibited in vivo efficacy that is much superior to vancomycin by eradicating bacteria and suppressing inflammation caused by MRSA-induced pneumonia in a rat model, demonstrating its promising therapeutic potential.
Leucine aminopeptidase (LAP) is a kind of proteolytic enzymes and associated closely with pathogenesis of cancer and liver injury. Accurate detection of LAP activity with high sensitivity and selectivity is imperative to detect its distribution and dynamic changes for understanding LAP's function and early diagnosing the disease states. However, fluorescent detection of LAP in living systems is challenging. To date, rarely fluorescent probes have been reported for imaging LAP in vivo. In this study, a novel probe (TMN-Leu) was developed by conjugating a near-infrared dicyanoisophorone derivative fluorophore with LAP activatable l-leucine amide moiety for the first time. TMN-Leu featured large Stokes shift (198 nm), favorable water solubility, ultrasensitive sensitivity (detection limit of ∼0.38 ng/mL), good specificity, excellent cell membrane permeability, low toxicity, and a prominent near-infrared emission (658 nm) in response to LAP. TMN-Leu has been successfully applied to track LAP of cancer cells and normal cells, monitor LAP changes in different disease models, and rapidly evaluate LAP inhibitor in cell-based assay. Notably, this probe firstly revealed that HCT116 cells with higher LAP activity were more invasive than LAP siRNA transfected HCT116 cells, suggesting that LAP might serve as an indicator reflecting the intrinsic invasion ability of cancer cells. Finally, TMN-Leu was also employed for in vivo real-time imaging LAP in living tumor-bearing nude mice with low background interference. All together, our probe possesses potential value as a promising tool for diagnostic application, cell-based screening inhibitors and in vivo real-time tracking enzymatic activity in preclinical applications.
We report non-volatile electric-field control of magnetism modulation in Fe/Pb(Mg1/3Nb2/3)0.7Ti0.3O3 (PMN-PT) heterostructure by fabricating an epitaxial Fe layer on a PMN-PT substrate using a molecular beam epitaxy technique. The remnant magnetization with a different electric field shows a non-symmetric loop-like shape, which demonstrates a change of interfacial chemistry and a large magnetoelectric coupling in Fe/PMN-PT at room temperature to realize low loss multistate memory under an electric field. Fitting with the angular-dependence of the in-plane magnetization reveals that the magnetoelectric effect is dominated by the direct electric-field effect rather than the strain effect at the interface. The magnetoelectric effect and the induced surface anisotropy are found to be dependent on the Fe film thickness and are linear with respect to the applied electric field.
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