RESUMEN
Oxygen evolution reaction (OER) is the key anode reaction of electrolytic water. To improve the slow OER kinetics, we synthesize nanoflower-like Co-Fe-Cr-Mo-Mn high-entropy spinel (HES) nanosheets on nickel foam (NF) by one-step solvothermal method, which exhibit an overpotential (η10) of only 188â mV at 10â mA cm-2, much lower than bimetallic CoFeOx/NF (233â mV), trimetallic CoFeCrOx/NF (211â mV), and tetrametallic CoFeCrMoOx/NF (200â mV). The OER overpotential decreases with the increase of the number of metals, indicating that the formation of HES has a positive effect on the improvement of electrocatalytic performance, since the synergistic effect between different metals enhances the charge transfer rate and decreases reaction barrier. In-situ Raman spectra demonstrate that the formation of γ-NiOOH on the HES surface is a crucial active species for the OER. This work demonstrates a simple and efficient synthesis method to prepare nanoflower-like high-entropy electrocatalysts for efficient OER electrocatalysis.
RESUMEN
TS-1 zeolite with desirable pore structure, an abundance of acidic sites, and good thermal stability promising as a support for the selective catalytic reduction of NO with NH3 (NH3-SCR). Herein, a series of Mn-Fe/TS-1 catalysts have been synthesized, adopting tetraethylenepentamine (TEPA) as a metal complexing agent using the one-pot hydrothermal method. The introduced TEPA can not only increase the loading of active components but also prompts the formation of a hierarchical structure through decreasing the size of TS-1 nanocrystals to produce intercrystalline mesopores during the hydrothermal crystallization process. The optimized Mn-Fe/TS-1(R-2) catalyst shows remarkable NH3-SCR performance. Moreover, it exhibits excellent resistance to H2O and SO2 at low temperatures. The characterization results indicate that Mn-Fe/TS-1(R-2) possesses abundant surface Mn4+ and Fe2+ and chemisorbed oxygen, strong reducibility, and a high Brønsted acid amount. For comparison, Mn-Fe/TiO2 displays a narrower active temperature window due to its poor thermostability.
RESUMEN
A new scheme of ion acceleration by crossing two ultraintense laser pulses in a near-critical relativistically transparent plasma is proposed. One laser, acting as a trigger, preaccelerates background ions in its radial direction via the laser-driven shock. Another crossed laser drives a comoving snowplow field which traps some of the preaccelerated ions and then efficiently accelerates them to high energies up to a few giga-electron-volts. The final output ion beam is collimated and quasimonoenergetic due to a momentum-selection mechanism. Particle-in-cell simulations and theoretical analysis show that the scheme is feasible and robust.
RESUMEN
A new regime in the interaction of a two-color (ω,2ω) laser with a nanometer-scale foil is identified, resulting in the emission of extremely intense, isolated attosecond pulses-even in the case of multicycle lasers. For foils irradiated by lasers exceeding the blow-out field strength (i.e., capable of fully separating electrons from the ion background), the addition of a second harmonic field results in the stabilization of the foil up to the blow-out intensity. This is then followed by a sharp transition to transparency that essentially occurs in a single optical cycle. During the transition cycle, a dense, nanometer-scale electron bunch is accelerated to relativistic velocities and emits a single, strong attosecond pulse with a peak intensity approaching that of the laser field.
RESUMEN
Shot-to-shot electron beam pointing instability in the plasma bubble, defined here as electron beam pointing jitter (EBJ), is a long-standing problem that limits the potential of the laser wakefield accelerator (LWFA) in a range of demanding applications. In general, EBJ is caused by variations in laser and plasma parameters from shot to shot, although the exact physical mechanism by which EBJ grows in the plasma wave remains unclear. In this work we theoretically investigate the fundamental physics of EBJ inside the plasma bubble and show how the intrinsic betatron oscillation can act as an amplifier to enhance EBJ growth. The analytical formulas for electron trajectory, pointing angle, and EBJ are derived from the basic momentum equation of an electron and verified numerically. It is shown that the shot-to-shot fluctuations of the laser and plasma parameters, such as laser strength, focus, and carrier-envelope phase, as well as the ambient plasma density and profile, lead to EBJ. The evolution of EBJ is dictated by the dynamics of the plasma bubble. Two amplification processes of the betatron oscillation are found in the rapidly evolving bubbles and play important roles in EBJ growth. The first is driven by a linear resonance in the wobbling bubble due to the coupling of the betatron oscillation and the bubble centroid oscillation. The second is a parametric resonance seen in the breathing bubble, where EBJ grows exponentially due to the strong frequency modulation of the betatron oscillation. Their characteristic functions, growth rates, and resonance conditions are deduced analytically and validated numerically. Finally, we also studied how radiation reaction affects EBJ. Our research provides a clear understanding of the basics of EBJ dynamics in LWFA and will help improve the use of LWFA in demanding applications.
RESUMEN
We report a novel cobalt-catalyzed intramolecular 1,4-hydrofunctionalization of dienes. The reaction proceeds under mild conditions and is amenable to N- and O-nucleophiles. The protocol exhibits exclusive regioselectivity, yielding a number of different alkenyl heterocycles, including but not limited to dihydroisobenzofurans, isochromanes, tetrahydrofurans, morpholines, lactones, and isoindolines. Experimental studies were performed to offer some insight into the different mechanistic pathways and to rationalize the regio- and stereoselectivities of the reaction.
RESUMEN
The increase in intense tropical cyclone (TC) activity across the western North Pacific (WNP) has often been attributed to a warming ocean. However, it is essential to recognize that the tropical WNP region already boasts high temperatures, and a marginal increase in oceanic warmth due to global warming does not exert a significant impact on the potential for TCs to intensify. Here we report that the weakened vertical wind shear is the primary driver behind the escalating trend in TC intensity within the summer monsoon trough of the tropical WNP, while local ocean surface and subsurface thermodynamic factors play a minor role. Through observational diagnoses and numerical simulations, we establish that this weakening of the vertical wind shear is very likely due to the increase in temperature of the Tibetan Plateau. With further warming of the Tibetan Plateau under the Representative Concentration Pathway 4.5 scenario, the projected TCs will likely become stronger.
RESUMEN
The development of high activity and strong resistance to seawater corrosion oxygen evolution reaction (OER) electrocatalysts for seawater electrolysis has broad application prospects. Herein, we prepare Co-doped FeNiOOH rosette-like nanoflowers on nickel foam (NF) with different Co dosages by one-step solvothermal method. The Co0.2-FeNiOOH/NF exhibits a low overpotential (η10) of 185 mV and Tafel slope of 30 mV dec-1 in 1 M KOH. Moreover, it shows a low η10 of 244 mV in alkaline seawater electrolyte. The remarkable OER performance of Co0.2-FeNiOOH/NF is ascribed to the fact that the introduction of Co regulates the morphology and electron structure of the material, which provides abundant active sites for the reaction and promotes charge transfer. In situ Raman results demonstrate that NiOOH and γ-FeOOH are the key active species for the OER. This study provides a feasible basis for seawater electrolysis over transition metal (oxy)hydroxides.
RESUMEN
High-entropy materials (HEMs) have potential application value in electrocatalytic water splitting because of their unique alloy design concept and significant mixed entropy effect. Here, we synthesize a high-entropy Ni-Fe-Cr-Mn-Co (oxy)hydroxide on nickel foam (NF) by a solvothermal method. The flower-like structure of FeNiCrMnCoOOH/NF can provide abundant active sites, thus improving the oxygen evolution reaction (OER) activity. In 1 M KOH, the FeNiCrMnCoOOH/NF shows an ultra-low overpotential (η10) of 201 mV for the OER, superior to FeNiCrMnAlOOH/NF, FeNiCrMnCuOOH/NF, FeNiCrMnMoOOH/NF, and FeNiCrMnCeOOH/NF. In addition, it exhibits a low η10 of 223 mV in 0.5 M NaCl + 1 M KOH and excellent stability. Electrochemical impedance spectroscopy measurements indicate that the synergistic effect between multiple metals accelerates charge transfer, while in situ Raman measurements reveal that NiOOH is a key active species for the OER. This work is of great significance for the construction of high-entropy (oxy)hydroxides for seawater electrolysis.
RESUMEN
Background: Percutaneous left atrial appendage (LAA) occlusion has been considered an efficient alternative to oral anticoagulation to prevent embolic events in patients with non-valvular atrial fibrillation (NVAF). Due to the complexities and heterogeneous anatomy of the LAA structure, the single-device approach may not always fit a large bilobulated LAA. This study aimed to evaluate the feasibility and safety of one-stop dual Watchman implantation for patients with bilobulated LAA. Methods: Included in the analysis were patients who underwent complete LAA closure with dual Watchman devices between December 2015 and December 2021. The anatomic morphology, procedure characteristics, procedure safety, and procedural complications were analyzed. Cardiac CT or transesophageal ultrasound was obtained at 7 days, 6 months, 1 year, and 2 years post-operatively to evaluate the effect of occlusion. Results: Among the 330 patients who underwent LAA occlusion during the study period, 7 (2.1%) patients were occluded with one-stop implantation of the double Watchman strategy. Successful occlusion was achieved in all patients. One patient had the double-access sheath strategy for implantation, and 6 patients had only a single-access sheath strategy for implantation. Pericardial effusion occurred in one case during the 7-day perioperative period. There was no device embolization, thrombosis, or obvious peridevice leakage (≥l mm) during the 2-year follow-up, with the exception of two cases with 2 mm of incomplete LAA sealing. Conclusion: The one-stop implantation of a dual Watchman is feasible and safe and might provide a strategy to occlude a large bilobulated LAA when incomplete closure is inevitable with a single device.