Electron Distribution Research Articles

Enhanced Adsorption Kinetics and Capacity of a Stable CeF3@Ni3N Heterostructure for Methanol Electro‐Reforming Coupled with Hydrogen Production

Alkaline methanol‐water electrolysis system is regarded as an appealing strategy for electro‐reforming methanol into formate and producing hydrogen with low energy‐consumption compared with alkaline water electrolysis. However, stability and selectivity under high current densities for practical application remain challenging. Herein, a CeF3@Ni3N nanosheets array anchored on carbon cloth (CeF3@Ni3N/CC) was fabricated. The gradual extrusion of F species from Ni(OH)2 lattices can stabilize hierarchical structure and construct abundant heterostructure interfaces. Moreover, CeF3 can modulate electron distribution of Ni3N, thus simultaneously enhancing the surface adsorption kinetics and capability of methanol and OH‐, which is conducive to enhanced methanol oxidation reaction (MOR) activity and selectivity. Therefore, bifunctional CeF3@Ni3N/CC exhibits low potential of 1.43 V at 500 mA cm‐2, along with high stability over 72 h and high faradaic efficiency (FEs) in MOR, as well as an overpotential of 76 mV to achieve 50 mA cm‐2 for hydrogen evolution reaction (HER). Furthermore, membrane‐free CeF3@Ni3N/CC||CeF3@Ni3N/CC cell for MOR||HER delivers high electrocatalytic activity, long‐term stability and FEs at high current density of 300 mA cm‐2. This study highlights the importance of optimizing surface adsorption behavior of active species, as well as rational design of highly efficient heterostructure electrocatalysts for methanol upgrading coupled with hydrogen production.

Enhanced Adsorption Kinetics and Capacity of a Stable CeF3@Ni3N Heterostructure for Methanol Electro‐Reforming Coupled with Hydrogen Production

Alkaline methanol‐water electrolysis system is regarded as an appealing strategy for electro‐reforming methanol into formate and producing hydrogen with low energy‐consumption compared with alkaline water electrolysis. However, stability and selectivity under high current densities for practical application remain challenging. Herein, a CeF3@Ni3N nanosheets array anchored on carbon cloth (CeF3@Ni3N/CC) was fabricated. The gradual extrusion of F species from Ni(OH)2 lattices can stabilize hierarchical structure and construct abundant heterostructure interfaces. Moreover, CeF3 can modulate electron distribution of Ni3N, thus simultaneously enhancing the surface adsorption kinetics and capability of methanol and OH‐, which is conducive to enhanced methanol oxidation reaction (MOR) activity and selectivity. Therefore, bifunctional CeF3@Ni3N/CC exhibits low potential of 1.43 V at 500 mA cm‐2, along with high stability over 72 h and high faradaic efficiency (FEs) in MOR, as well as an overpotential of 76 mV to achieve 50 mA cm‐2 for hydrogen evolution reaction (HER). Furthermore, membrane‐free CeF3@Ni3N/CC||CeF3@Ni3N/CC cell for MOR||HER delivers high electrocatalytic activity, long‐term stability and FEs at high current density of 300 mA cm‐2. This study highlights the importance of optimizing surface adsorption behavior of active species, as well as rational design of highly efficient heterostructure electrocatalysts for methanol upgrading coupled with hydrogen production.

Application of a large wall electric probe (LWEP) for plasma and ambient gas studies

Abstract The operation of a large wall electric probe (LWEP) is analyzed, where the probe surface area in contact with the plasma is only a few times smaller than the area of the plasma boundaries. Compared to a small standard Langmuir probe (SLP), the LWEP may have significantly greater resolution and sensitivity, but could substantially perturb the plasma and distort the measured properties. A target application for the LWEP is where the sensitivity of the measurement is critical, but the effects of the plasma perturbation is minimal. A specific case where a LWEP may outperform a SLP is the measurement of a nonlocal electron distribution function at energies of electron free diffusion, that is, at energies significantly exceeding thermal electron energies, in order to obtain information about the parameters of the plasma or ambient gas. Examination of the LWEP analysis process has revealed that, depending on the plasma volume and probe configurations, it may be necessary to measure either the first or second derivatives of the probe current with respect to the probe potential to derive the energetic part of the electron energy distribution function.

Lewis acid sites in hollow cobalt phytate micropolyhedra promote the electrocatalytic water oxidation.

The acid-base microenvironment of the metal center is crucial for constructing advanced oxygen evolution reaction (OER) electrocatalysts. However, the correlation between acidic site and OER performance remains unclear for cobalt-based catalysts. Herein, Lewis acid sites in hollow cobalt phytate micropolyhedra (M-CoPA, M = Cu, Sr) were synthesized by a cation-exchange strategy, and their OER performances were studied systematically. Experimentally, Lewis acid Cu2+ sites with stronger Lewis acidity exhibited superior intrinsic activity and long-term stability in alkaline electrolytes. The spectroscopic and electrochemical studies show Lewis acid sites in hollow cobalt phytate micropolyhedra can modulate the electronic distribution of the adjacent cobalt center and further optimize the adsorption strength of oxygenated species. This study figures out the effect of Lewis acid sites on the OER kinetics and provides an effective way to develop high-efficiency electrocatalysts for energy conversion systems.

In-Situ Constructing N,S-Codoped Carbon Heterointerface for High-Rate Cathode of Sodium-Ion Batteries.

Na3V2(PO4)3 (NVP) is considered one of the promising choices for cathodes of sodium-ion batteries, but the poor conductivity resulted inferior rate performance limited the practical development of NVP cathodes. In this study, we successfully synthesized N/S dual-atom doped carbon coatings in situ through a simple one-step solid-state sintering method. The uniformly coated carbon layer can inhibit the agglomeration and growth of active materials during the sintering process, shorten the Na+ migration path, and increase the contact area with the electrolyte, thus facilitating rapid Na+ migration. Notably, the doping of N elements can alter the electron distribution of carbon coating, enhancing electron conductivity. Furthermore, the introduction of S elements in the carbon layer can induce the formation of stable C-S-C bonds in the molecular layer, expanding the interlayer spacing, which is beneficial for Na+ transport and storage. Therefore, the modified NVP@NSC composite provides a high specific capacity of 90.3 mAh g-1 at a rate of 20 C, with a capacity retention rate of 94.4% after 8000 cycles, demonstrating excellent stability at high current densities. Moreover, the full cell exhibits remarkable electrochemical performance at 5 C. This research contributes to the practical development of NVP cathodes.

Cross-calibration and first vertical ECE measurement of electron energy distribution in the TCV tokamak

Abstract This paper describes the first vertical electron cyclotron emission measurement of non-thermal electron distributions in the Tokamak à Configuration Variable. These measurements were conducted in runaway electron scenarios and in the presence of electron cyclotron current drive. Measured intensities of linearly polarized X- and O-mode radiation from fast electrons allow the analysis of the energy distribution. The measurements were made possible through the creation of an operational regime for the diagnostic that is free of thermal background radiation, in relaxed electron density operations. This operational regime notably enables the cross-calibration of the diagnostic system, relying on thermal plasma measurements and modeling with the ray-tracing code SPECE.

Synchrotron Polarization of a Hybrid Distribution of Relativistic Thermal and Nonthermal Electrons in Gamma-Ray Burst Prompt Emission

Synchrotron polarization of relativistic nonthermal electrons in gamma-ray bursts (GRBs) has been widely studied. However, recent numerical simulations of relativistic shocks and magnetic reconnection have found that a more realistic electron distribution consists of a power-law component plus a thermal component, which requires observational validation. In this paper, we investigate synchrotron polarization using a hybrid energy distribution of relativistic thermal and nonthermal electrons within a globally toroidal magnetic field in GRB prompt emission. Our results show that compared to the case of solely nonthermal electrons, the synchrotron polarization degrees (PDs) in these hybrid electrons can vary widely, depending on different parameters, and that the PD decreases progressively with frequency in the gamma-ray, X-ray, and optical bands. The time-averaged PD spectrum displays a significant bump in the gamma-ray and X-ray bands, with the PDs higher than ∼60% if the thermal peak energy of the electrons is much smaller than the conjunctive energy of the electrons between the thermal and nonthermal distributions. The high-synchrotron PDs (≳60%) in the gamma-ray and X-ray bands, which generally cannot be produced by solely nonthermal electrons with typical power-law slopes, can be achieved by hybrid electrons and primarily originates from the exponential decay part of the thermal component. Moreover, this model can roughly explain the PDs and spectral properties of some GRBs, where GRB 110301A with a high PD ( 70−22+22% ) may be potential evidence for the existence of relativistic thermal electrons.

Analysis of the high-temperature transport property in GaN-based single and double heterostructures

GaN-based heterostructures have been proved to be excellent candidates for high-voltage, large-power, high-frequency and high-temperature application fields, thanks to their superior material properties. To further improve the carriers’ confinement, using InGaN channel layer or introducing AlGaN back barrier layer is promoted. These structures are also proved to be favorable for the robust electron mobility at high temperature. However, the reason solely rests on the longitudinal optical (LO) phonon scattering and the behind mechanism is still absent. This work compares the temperature-dependent electronic transport properties in three groups of GaN-based heterostructures, including GaN-based single heterostructure (SH) with/without AlN interlayer, GaN-based SH and double heterostructure (DH), and GaN-based DH with AlGaN or GaN channel layer. The advantageous high-temperature mobility is attributed to the enhanced LO phonon energy in heterostructures. By self-consistent calculations of the Schrödinger–Poisson equations, a close relation between the narrow electron distribution in the quantum well with the high LO phonon energy, and consequently superior mobility at high temperature is implied. The results provide a simple strategy for the optimized design of the GaN-based heterostructures outperforming at high temperature.

Electron Energization by Ion Density Enhancement in the Martian Magnetotail—MAVEN Observations

It has been long observed at Mars that electron fluxes are enhanced during the tail current sheet crossings, of which the cause is not well understood. We use a novel approach to reveal one of the electron energization mechanisms with observations from the Mars Atmospheric and Volatile EvolutioN (MAVEN) mission. We find the field-aligned potential, derived from comparing electron distribution functions, to be approximately linearly correlated with the logarithmic values of the local total ion density. This is the expected behavior of an ambipolar electrostatic potential. The large amplitude of potential (tens to hundreds of V) is a result of both a significant density gradient (1 order of magnitude) and the high electron temperature (tens of eV) in the tail. Such a mechanism is not limited to ion density enhancements at current sheet crossings but can be present anywhere that large ion density gradients and hot electrons are present.

Calculating a perturbation of a plasma layer by an electric field

The paper presents the results of solving a boundary value problem for a system of two integro-differential equations that simulate the action of an external electric field on a plasma layer. This system is an implication of the Boltzmann–Maxwell equations, and the physical meaning of the sought functions is the strength of a self-consistent electric field and perturbation of the electron distribution density. The solution of the problem is constructed using the theories of Fourier transform of generalized functions and singular integral equations with the Cauchy kernel. The dependence of the solution on the frequency of the external field is studied.

Exploring the Correlation Between the Molecular Structure and Biological Activities of Metal–Phenolic Compound Complexes: Research and Description of the Role of Metal Ions in Improving the Antioxidant Activities of Phenolic Compounds

We discussed and summarized the latest data from the global literature on the action of polyphenolic antioxidants and their metal complexes. The review also includes a summary of the outcomes of theoretical computations and our many years of experimental experience. We employed various methods, including spectroscopy (FT-IR, FT-Raman, NMR, UV/Vis), X-ray diffraction, thermal analysis, quantum calculations, and biological assays (DPPH, ABTS, FRAP, cytotoxicity, and genotoxicity tests). According to our research, the number and position of hydroxyl groups in aromatic rings, as well as the delocalization of electron charge and conjugated double bonds, have a major impact on the antioxidant effectiveness of the studied compounds. Another important factor is metal complexation, whereby high ionic potential metals (e.g., Fe(III), Cr(III), Cu(II)) enhance antioxidant properties by stabilizing electron charge, while the low ionic potential metals (e.g., Ag(I), Hg(II), Pb(II)) reduce efficacy by disrupting electron distribution. However, we observed no simple correlation between ionic potential and antioxidant capacity. This paper gives insights that will aid in identifying new, effective antioxidants, which are vital for nutrition and the prevention of neurodegenerative illnesses. Our results outline the connections between biological activity and molecular structure, offering a foundation for the methodical design of antioxidants. Our review also shows in detail how we use various complementary methods to assess the impact of metals on the electronic systems of ligands. This approach moves beyond the traditional “trial and error” method, allowing for the more efficient and rational development of future antioxidants.

Modifying d–p orbital hybridization of Ni/Fe[sbnd]O species by high-valence ruthenium doping to enhance oxygen evolution performance

The electron distribution of catalysts can be modulated by high-valence metal doping, thus enhancing the intrinsic activity. Herein, we adopt Ru modification to adjust the d–p orbital hybridization of Ni-Fe oxyhydroxides, significantly increasing the oxygen evolution reaction (OER) activity. The amorphous NiFe0.5Ru0.1OxHy catalyst synthesized by sol–gel method exhibits excellent OER activity, far superior to commercial RuO2. In situ Raman and XPS results confirm that the NiOOH/FeOOH active species gradually form with increasing applied voltage. Density functional theory (DFT) calculations reveal that high-valence Ru dopants can effectively regulate the hybridization of d–p orbital of Ni/FeO, significantly increase the electron density around Fermi level, promote charge transfer, make them have more anti-bonding orbitals, enhance the binding ability of active sites to intermediates, reduce the reaction energy barrier of the rate-determining step (H2O → *OH), and thus improve the OER activity. In addition, NiFeRuOxHy as a cathode catalyst in a rechargeable zinc-air battery shows an outstanding cycle life of 600 h. This study provides a promising hybrid orbital method for designing high-performance OER catalysts for water splitting and rechargeable zinc-air batteries.

Monte Carlo modeling of the origin of contaminant electrons on a 0.5T bi-planar Linac-MR.

In the last decade, hybrid linear accelerator magnetic resonance imaging (Linac-MR) devices have evolved into FDA-cleared clinical tools, facilitating magnetic resonance guided radiotherapy (MRgRT). The addition of a magnetic field to radiation therapy has previously demonstrated dosimetric and electron effects regardless of magnetic field orientation. This study uses Monte Carlo simulations to investigate the importance and efficacy of the magnetic field design in mitigating surface dose enhancement in the Aurora-RT, focusing specifically on contaminant electrons, their origin, and energy spectrum. The Aurora-RT 0.5 T Biplanar Linac-MR device was modeled using the BEAMnrc package using the updated EM macros, a magnetic field map generated from Opera 3D. Simulation generated phasespace data at the distal side of the first magnetic pole plate (89cm) and at machine isocenter (120cm) were analyzed with respect to electron energy spectra and electron creation origins, both with and without the static magnetic field. The presence of the main magnetic field was verified to affect the origin and distribution of contaminant electrons, removing them from the air column up to 60cm from the target, and focusing them along the CAX within the region below. Analysis of the remaining electron energy fluence reveals the net removal of electrons with energies>2 MeV and generation of electrons with energies<2 MeV in the presence of the static magnetic field as compared to no magnetic field. Moreover, in the presence of the magnetic field the integral energy contained in the contaminant electrons increases from 89cm to isocenter but is still 15% less overall than the integral energy contained in contaminant electrons without the magnetic field. This study provides an analysis of contaminant electrons in the Aurora-RT 0.5 T Linac-MR, emphasizing the role of magnetic field design in successfully minimizing electron contaminants.

Efficient photocatalytic degradation of methylene blue via synergistic dual co-catalyst on SrTiO3@Al under visible light: Experimental and DFT study

BackgroundPhotocatalytic oxidation is a green method for water purification. However, the operation of traditional photocatalysts depends on exposure to UV radiation, which only forms a small portion of the spectrum comprising sunlight. The expansion of photocatalyst absorption to the visible range of light could greatly improve the efficiency and economic viability of the process. MethodsThe photocatalyst was prepared by first synthesising SrTiO3 nanoparticles by chemical precipitation followed by calcination. Then, SrTiO3 was doped with aluminium using a flux method with Al2O3 and SrCl2 at 1150 °C. Finally, the dual co-catalysts, Rh/Cr2O3 and CoOOH, were photodeposited onto SrTiO3@Al via sequential irradiation. Significant findingsThe Rh/Cr2O3/SrTiO3@Al/CoOOH nanocomposite degraded 87% of methylene blue (MB) (10 mg/L) under visible light in 1 h, a 3.3-fold improvement over pure SrTiO3 and 2.1-fold over a similar commercial composite. This enhancement is due to efficient charge separation resulting from Al doping and improved carrier transport as a result of the anisotropic deposition of the co-catalysts. Optimisation showed that 20 mg of photocatalyst in 50 mL of MB solution (5 mg/L) degraded 100% thereof within 45 min. DFT calculations showed uneven electron distribution in SrTiO3′s conduction band and structural changes with Al doping, further enhancing photocatalytic activity.

Triggering Ion Diffusion and Electron Transport Dual Pathways for High Efficiency Electrochemical Li+ Extraction.

Efficient electrochemical Li+ adsorption holds significant promise for lithium extraction, while the mismatched rate between Li+ diffusion and electron transport within the electrode material impedes the electrochemical activity and restricts the adsorption efficiency. To address this challenge, herein, we rationally design and integrate the ion and electron dual-conducting poly(vinyl alcohol)-polyaniline (PVA-PANI) copolymer (CP) within the H1.6Mn1.6O4 (HMO) electrode matrix to facilitate Li+ diffusion and electron transport. The Li+ diffusion coefficient (DLi+) increased from 3.03 × 10-10 to 5.92 × 10-10 cm2/s, while the charge transfer resistance (Rct) decreased from 53.73 to 29.57 ohm. Consequently, the HMO@CP electrode exhibits superior adsorption kinetics and a state-of-the-art high adsorption capacity of up to 49.48 mg/g. Comprehensive mechanistic studies reveal that the negatively charged hydroxyl groups (-OH) in PVA accelerate Li+ diffusion and that the conjugated structure and redox-active quinoid sites in PANI offer denser electron distribution and promote electron transport. This synergistic effect in CP significantly enhanced Li+ diffusion and electron transport, leading to electrochemical activity and adsorption efficiency. Our work highlights the critical role of simultaneously regulating the ion diffusion and electron transport dual pathways for optimizing Li+ adsorption performance and inspires development of the next generation electrochemical adsorption electrodes.

Synthesis, Characterization, and Therapeutic Potential of Novel Schiff Base Metal Complexes: Nickel(II) and Copper(II) Complexes Based 2‐[(2‐Chloroquinolin‐3‐yl)methylidene]aminobenzenethiol (CQAT)

ABSTRACTThis research focused on the design and comprehensive characterization of two novel transition metal complexes derived from the symmetrical Schiff base 2‐[(2‐chloroquinolin‐3‐yl)methylidene]aminobenzenethiol (CQAT), coordinated with nickel(II) (NiCQAT) and copper(II) (CuCQAT) ions. The structural elucidation of these complexes was achieved through a range of advanced analytical techniques. Thermal analysis revealed the stability and decomposition patterns of the complexes, supporting the identification of their coordination geometries. The collective data indicated that both NiCQAT and CuCQAT complexes adopt octahedral coordination, with the specific formulas [Ni(CQAT)2(H2O)2] and [Cu(CQAT)2(H2O)2], respectively. To complement the experimental findings, density functional theory (DFT) calculations were employed. These theoretical calculations confirmed the proposed molecular structures and provided detailed insights into key quantum chemical parameters, such as HOMO–LUMO energies, molecular orbitals, and electronic distributions, which are crucial for understanding the complexes' reactivity and stability. Furthermore, extensive in vitro biological evaluations were conducted to assess the anti‐inflammatory and antioxidant properties of the synthesized complexes. These assays demonstrated that both NiCQAT and CuCQAT exhibited significantly enhanced bioactivity compared to the free CQAT ligand, suggesting a synergistic effect of metal coordination on the ligand's biological efficacy. To further explore the mode of action, molecular docking studies were performed targeting two key proteins—human cyclooxygenase‐2 (PDB ID: 5IKT) and human peroxiredoxin 2 (PDB ID: 5IJT). The docking simulations provided valuable insights into the binding affinities, interaction energies, and key amino acid residues involved in the binding process, offering a molecular‐level understanding of their potential biological mechanisms. The findings from these multidisciplinary studies highlight the therapeutic potential of CQAT and its nickel and copper complexes, positioning them as promising candidates for further development in the field of medicinal chemistry.

Understanding and Mastering Multiphysical Fields Toward Dendrite‐Free Aqueous Zinc Batteries

AbstractAqueous zinc batteries (AZBs) have emerged as promising candidates for next‐generation grid‐scale energy storage due to their excellent safety, environmental friendliness, and abundance of Zn metal. However, undesired dendrite growth on Zn anodes, resulting from uneven Zn plating/stripping, leads to poor durability and low Coulombic efficiency, posing significant challenges for the practical application of AZBs. Multiple physical fields, the intrinsic driving force governing the distribution of electrons and ions, significantly impact Zn deposition behavior. The underlying mechanisms and regulation strategies related to this phenomenon has not been fully reviewed. This comprehensive review focuses on revealing the key physical fields influencing Zn deposition (including ionic flux, electric field, stress field, and temperature field) and summarizes the most effective control methods. Each approach is thoroughly scrutinized, highlighting its operational mechanisms, benefits, and limitations. Furthermore, the challenges and potential pathways for developing durable Zn anodes are outlined. Through in‐depth analysis of the influences of multiphysical fields on Zn deposition behavior, this review sets the foundation for enhancing the performance of Zn anodes, thereby supporting the advancement of Zn batteries commercialization.

Electron Acceleration in Magnetic Islands in Quasi-parallel Shocks

We report new theories and simulations for electron acceleration in magnetic islands generated by magnetic reconnection in the shock turbulence in a quasi-parallel shock, using a 2 and 1/2 dimensional particle-in-cell simulation. When an island is moving, unmagnetized electrons are accelerated by the Hall electric field pointing toward the island center. In a stationary island, some electrons are energized by “island betatron acceleration” due to the induction electric field when the island core magnetic field changes with time. In the simulation, almost all of the high-energy electrons in the shock transition region that show a power-law distribution are accelerated in ion-skin-depth-scale magnetic flux ropes, and about half of them are accelerated by the Hall electric field and island betatron acceleration. These mechanisms can produce a power-law electron distribution, and also inject electrons into the diffusive shock acceleration. The mechanisms are applicable to quasi-parallel shocks with high Alfvén Mach numbers (M A > 10), including planetary bow shocks and shocks in astrophysical objects such as supernova remnants.

Exploring Unconventional Electron Distribution Patterns: Contrasts Between FeSe and FeSe/STO Using an Ab Initio Approach

For more than a decade, the unusual distribution of electrons observed in ARPES (angle-resolved photoemission spectroscopy) data within the energy range of ~30 meV to ~300 meV below the Fermi level, known as the ARPES energy range, has remained a puzzle in the field of iron-based superconductivity. As the electron–phonon coupling of FeSe/SrTiO3 is very strong, our investigation is centered on exploring the synergistic interplay between spin-density waves (SDW) and charge-density waves (CDW) with differential phonons at the interface between antiferromagnetic maxima and minima under wave interference. Our analysis reveals that the synergistic energy is proportional to the ARPES energy range, as seen in the comparison between FeSe and FeSe/SrTiO3. This finding may suggest that the instantaneous interplay between these intricate phenomena may play a role in triggering the observed energy range in ARPES.

Enhancing the Filler Utilization of Composite Gel Electrolytes via In Situ Solution-Processable Method for Sustainable Sodium-Ion Batteries.

The composite gel electrolyte (CGE), which combines the advantages of inorganic solid-state electrolytes and solid polymer electrolytes, is regarded as the ultimate candidate for constructing batteries with high safety and superior electrode-electrolyte interface contact. However, the ubiquitous agglomeration of nanofillers results in low filler utilization, which seriously reduces structural uniformity and ion transport efficiency, thus restricting the development of consistent and durable batteries. Herein, a solution-processable method to in situ construct CGE with high filler utilization is introduced. The homogeneous metal-organic framework fillers contribute to uniform ionic and electronic filed distribution, realizing a stable electrode-electrolyte interface. Consequently, the CGE with high filler utilization achieves an ultra-long lifespan of 10000 cycles with a capacity retention of 80.2%. This work provides guidance for constructing high-performance CGEs in electrochemical energy-storage devices.