Atomic Capture Research Articles

Rapid oxygen atom capture on perovskite surface boosting the activity and durability of cathode for solid oxide fuel cells

The content and distribution of surface oxygen vacancies are crucial for the oxygen reduction reaction (ORR) activity of solid oxide fuel cell (SOFC) cathodes. Therefore, a facile and rapid oxygen atom capture strategy is developed to modulate the surface oxygen vacancies of the cathode. By controlling the duration of NaBH4 solution reduction, precise modulation of the surface oxygen vacancies of NdBa0.5Sr0.5Co2O5+δ (NBSC) is achieved. Consequently, the processes of oxygen adsorption, dissociation, and diffusion on the surface of the NBSC cathode are enhanced. The research findings demonstrate that NBSC reduced for 10 min (RE-NBSC-10) exhibits optimal ORR catalytic activity and CO2 tolerance. At 800 °C, the Rp of RE-NBSC-10 decreases by 45 %, reaching 0.006 Ω‧cm2. Moreover, the maximum power density (MPD) of the RE-NBSC-10 cathode reaches 1.16 W cm−2, representing a 90.2 % improvement compared to NBSC. This research provides an efficient approach for the advancement of materials tailored for next-generation energy conversion devices.

Precise construction of RuPt dual single-atomic sites to optimize oxygen electrocatalytic behaviors for high-performance Zn-air batteries

The development of redox bifunctional electrocatalysts with high performance, low cost, and long lifetimes is essential for achieving clean energy goals. This study proposed an atom capture strategy for anchoring dual single atoms (DSAs) in a zinc–zeolitic imidazolate framework (Zn–ZIF), followed by calcination under an N2 atmosphere to synthesize ruthenium–platinum DSAs supported on a nitrogen-doped carbon substrate (RuPt DSAs-NC). Theoretical calculations showed that the degree of Ru 5dxz − *O 2px orbital hybridization was high when *O was adsorbed at the Ru site, indicating enhanced covalent hybridization of metal sites and oxygen ligands, which benefited the adsorption of intermediate species. The presence of the RuPtN6 active center optimized the absorption–desorption behavior of intermediates, improving the electrocatalytic performance of the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER). RuPt DSAs-NC exhibited a 0.87 V high half-wave potential and a 268 mV low overpotential at 10 mA cm−2 in an alkaline environment. Furthermore, rechargeable zinc–air batteries (ZABs) achieved a peak power density of 171 mW cm−2. The RuPt DSAs-NC demonstrated long-term cycling for up to 500 h with superior round-trip efficiency. This study provided an effective structural design strategy to construct DSAs active sites for enhanced electrocatalytic performance.

Hydrogen trapping behavior in IVB-VB transition metal carbides

The hydrogen capture mechanism of transition metal carbides is crucial to improve the hydrogen embrittlement resistance of steel materials. Although numerous experimental and theoretical studies have been carried out, the mechanism of hydrogen capture in these carbides has not been fully elucidated. In this paper, the ability of transition metal carbides (TMCs; TM=Ti, Zr, Hf, V, Nb and Ta) to capture hydrogen is studied by first-principles calculations. It is found that there is a strong correlation between the hydrogen solubility energy and the number of valence electrons of IV-VB transition metal carbides. With the increase of the number of valence electrons, the hydrogen solubility energy decreases, which indicates that IVB transition metal carbides have strong hydrogen capture ability. Compared with interstitial sites, the mechanism by which carbon vacancies are more stable hydrogen capture sites is to enhance the capture stability of hydrogen atoms by reducing the effect of chemical and mechanical effects on the dissolution energy of hydrogen atoms. In the interstitial site, hydrogen atoms tend to occupy the triangular site (TMCs-TM) surrounded by three transition metal atoms and one carbon atom. The bonding interaction between the hydrogen atom and the nearest carbon atom is the main factor affecting the stability of hydrogen atom capture.

Pd(II)/Pd(IV) redox shuttle to suppress vacancy defects at grain boundaries for efficient kesterite solar cells

Charge loss at grain boundaries of kesterite Cu2ZnSn(S, Se)4 polycrystalline absorbers is an important cause limiting the performance of this emerging thin-film solar cell. Herein, we report a Pd element assisted reaction strategy to suppress atomic vacancy defects in GB regions. The Pd, on one hand in the form of PdSex compounds, can heterogeneously cover the GBs of the absorber film, suppressing Sn and Se volatilization loss and the formation of their vacancy defects (i.e. VSn and VSe), and on the other hand, in the form of Pd(II)/Pd(IV) redox shuttle, can assist the capture and exchange of Se atoms, thus contributing to eliminating the already-existing VSe defects within GBs. These collective effects have effectively reduced charge recombination loss and enhanced p-type characteristics of the kesterite absorber. As a result, high-performance kesterite solar cells with a total-area efficiency of 14.5% (certified at 14.3%) have been achieved.

Capture of single Ag atoms through high-temperature-induced crystal plane reconstruction

The “terminal hydroxyl group anchoring mechanism” has been studied on metal oxides (Al2O3, CeO2) as well as a variety of noble and transition metals (Ag, Pt, Pd, Cu, Ni, Fe, Mn, and Co) in a number of generalized studies, but there is still a gap in how to regulate the content of terminal hydroxyl groups to influence the dispersion of the active species and thus to achieve optimal catalytic performance. Herein, we utilized AlOOH as a precursor for γ-Al2O3 and induced the transformation of the exposed crystal face of γ-Al2O3 from (110) to (100) by controlling the calcination temperature to generate more terminal hydroxyl groups to anchor Ag species. Experimental results combined with AIMD and DFT show that temperature can drive the atomic rearrangement on the (110) crystal face, thereby forming a structure similar to the atomic arrangement of the (100) crystal face. This resulted in the formation of more terminal hydroxyl groups during the high-temperature calcination of the support (Al-900), which can capture Ag species to form single-atom dispersions, and ultimately develop a stable and efficient single-atom Ag-based catalyst.

Reverse Atom Capture on Perovskite Surface Enabling Robust and Efficient Cathode for Protonic Ceramic Fuel Cells.

Protonic ceramic fuel cells (PCFCs) hold potential for sustainable energy conversion, yet their widespread application is hindered by the sluggish kinetics and inferior stability of cathode materials. Here, a facile and efficient reverse atom capture technique is developed to manipulate the surface chemistry of PrBa0.5Sr0.5Co1.5Fe0.5O5+ δ (PBSCF) cathode for PCFCs. This method successfully captures segregated Ba and Sr cations on the PBSCF surface using W species, creating a (Ba/Sr)(Co/Fe/W)O3- δ (BSCFW)@PBSCF heterostructure. Benefiting from enhanced kinetics of proton-involved oxygen reduction reaction and strengthened chemical stability, the single cell using the optimized 2W-PBSCF cathode demonstrates an exceptional peak power density of 1.32W cm-2 at 650°C and maintains durable performance for 240h. Theoretical calculations unveil that the BSCFW perovskite delivers lower oxygen vacancy formation energy, hydration energy, and proton transfer energy compared to the PBSCF perovskite. This protocol offers new insights into advanced atom capture techniques for sustainable energy infrastructures.

High flux strontium atom source

We present a novel cold strontium atom source designed for quantum sensors. We optimized the deceleration process to capture a large velocity class of atoms emitted from an oven and achieved a compact and low-power setup capable of generating a high atomic flux. Our approach involves velocity-dependent transverse capture of atoms using a two-dimensional magneto-optical trap. To enhance the atomic flux, we employ tailored magnetic fields that minimize radial beam expansion and incorporate a cascaded Zeeman-slowing configuration utilizing two optical frequencies. The performance is comparable to that of conventional Zeeman slower sources, and the scheme is applicable to other atomic species. Our results represent a significant advancement towards the deployment of portable and, possibly, space-based cold atom sensors.

Numerical Modeling of the Interaction of Dark Atoms with Nuclei to Solve the Problem of Direct Dark Matter Search

The puzzle of the direct dark matter search can be resolved by examining the concept of «dark atoms», which consist of hypothetical stable lepton-like particles with a charge of −2n, where n is any natural number, bound to n nuclei of primordial helium. These «dark atoms», known as «XHe» (X-helium) atoms, remain undiscovered in experiments due to their neutral atom-like states. In this model, the positive results of the DAMA/NaI and DAMA/LIBRA experiments could be explained by the annual modulation of radiative capture of XHe atoms engaging in low-energy bound states with sodium nuclei. This specific phenomenon does not occur under the conditions of other underground experiments. The proposed solution to this puzzle involves establishing the existence of a low-energy bound state of «dark atoms» and nuclei while also considering the self-consistent influence of nuclear attraction and Coulomb repulsion. Resolving this complex issue, which has remained unsolved for the past 17 years, necessitates a systematic approach. To tackle this problem, numerical modeling is employed to uncover the fundamental processes behind the interaction of «dark atoms» with nuclei. To comprehend the essence of XHe’s interaction with baryonic matter nuclei, a classical model is employed wherein quantum physics and nuclear size effects are progressively incorporated. A numerical model describing the interaction between XHe «dark atoms» and nuclei is developed through the continuous inclusion of realistic features of quantum mechanics in the initial classical three-body problem involving the X-particle, the helium nucleus, and the target nucleus. This approach yields a comprehensive numerical model that encompasses nuclear attraction and electromagnetic interaction between the «dark atom» and nuclei. Finally, this model aids in supporting the interpretation of the results obtained from direct underground dark matter experiments through the lens of the «dark atom» hypothesis.

Strong atom capture ability and pinning effect by doping an element with large electronegativity difference in Sb2Te3 phase change material

The ultimate goal of memory researchers and developers is to devise a universal memory to replace all memories in complex hierarchies of memory systems. Phase change memory is considered by the International Semiconductor Industry Association as the most likely emerging storage technology to achieve this ambitious goal due to its excellent performance. However, the relatively slow operation speed and poor cycle endurance are stumbling blocks for this purpose. Here, we propose a new doping strategy to construct stable bonding by introducing atoms with large electronegativity differences from the matrix Te atoms enhancing the capture ability and the pinning effect to Te atoms, which facilitates fast nucleation and suppresses migration of Te atoms to achieve significant performance improvement. Using ab initio molecular dynamics simulations, we explore and compare the atomic structures, chemical bonding, and dynamics properties of Hf doped Sb2Te3 (HfST), La doped Sb2Te3 (LaST), Rb doped Sb2Te3 (RbST) and Sr doped Sb2Te3 (SrST). In the XST (X refers to Hf, Rb, La and Sr atoms) systems, the increase of the more stable ring structure fluctuation and the stronger atom capture capability of rings enable more and faster formation of nuclei during crystallization. Higher Peierls-like distortions suggest better thermal stability. The motility of Te atoms is suppressed due to the pinning effect. High coordination of atoms and the concentration reduction of the lone-pair electron and void enable small density difference. Our results show that fast universal memory with good endurance can be achieved by the construction of strong bonding by doping atoms with large electronegativity differences, providing an important guidance for experiments and industries.

FORMATION AND DECOMPOSITION OF ANOMALOUS SUPERSATURATED MOLYBDENUM SOLUTIONS IN COPPER-BASED CONDENSATES


 Cu-Mo condensates in the concentration range of the latter from 0.3 to 1.5 at.%, obtained by simultaneous evaporation in vacuum with subsequent condensation of the resulting vapor mixture on a non-orienting substrate (PVD method), were studied. The components of this system do not form chemical compounds under equilibrium conditions and are mutually insoluble in liquid and solid states. The structure of Cu-Mo condensates was studied by transmission electron microscopy and X-ray diffractometry both in the derivative state and after a series of isothermal anneals in the temperature range from 300 to 900°C. It was found that small concentrations of molybdenum lead to significant dispersion of the matrix metal. Molybdenum tends to form segregations at the boundaries of copper grains and form a strong coherent bond with the matrix metal, which persists even after isothermal annealing. The conditions for the formation of an anomalous supersaturated solid solution of molybdenum in the copper matrix, as well as the conditions for its decomposition, have been revealed. An assumption is made about the mechanism of formation of such a solution during condensation from the vapor phase, which consists in the kinetic capture of molybdenum atoms by the crystallization front during condensation from the vapor phase. It was found that the decomposition of the supersaturated solid solution begins when heated to 0.5 of the melting point of copper and is accompanied by a dispersion solidification process. During the experiment, it was first recorded that the dispersion solidification process can have a two-stage character. The first peak is observed in the region of 30 minutes of annealing, and the second peak is observed after about 2 hours of isothermal annealing. The height of the dispersion hardening peaks increases with increasing molybdenum concentration. It is suggested that the appearance of the second peak of dispersion hardening is associated with the peculiarities of the interaction between copper grains and molybdenum segregations at the grain boundaries. It is shown that the structure after solution decomposition is typically composite. The advantage of this material over conventional dispersively hardening alloys is the fact that in these pseudo-alloys there is no reverse solution of hardening particles at an increase in temperature.

Magnetization properties of radially polarized Bessel-Gaussian vortex beams with radial phase modulation in a 4π focusing system.

This paper explored the optically induced magnetization properties of radially polarized Bessel-Gaussian vortex beams with radial phase modulation in a 4π high numerical aperture (NA) focusing system, which is based on the vector diffraction theory and the inverse Faraday effect. The results show that in the case of radial modulation parameter L=0, one longitudinal magnetization chain with adjustable length can be obtained by modulating the truncation parameter β. When the radial modulation parameter L=1.3, two magnetization chains can be obtained by modulating the truncation parameter β. By modulating the radial modulation parameter L, two magnetization chains along the optical axis can be generated, each with four dark magnetic traps; meanwhile, the spacing between two magnetization chains can be adjusted. These results may be helpful in high-density all-optical magnetic recording, atom capture, and magnetic resonance microscopy.

Self-consistent calculations for atomic electron capture

Self-consistent calculations for atomic electron capture

Effects of hydrogen on passivation and semiconductive properties of passive film on Fe-based amorphous coatings

Hydrogen atoms accumulate in the grain boundaries, dislocations and twins of metals, but the Fe-based amorphous coatings do not have these crystal defects. The effect of hydrogen on the passivation and semiconductive properties could provide a theoretical support for the application of Fe-based amorphous coatings at high hydrogen concentrations. The passivation and semiconductive properties of passive film on plasma-sprayed Fe-based amorphous coatings were investigated via electrochemical impedance spectroscopy combined with a point defect model. The phase compositions of the passive films were verified via X-ray photoelectron spectroscopy. The morphology of the coatings and the surface state of the passive films were characterized via scanning electron microscopy and atomic force microscopy. Finally, the long-time hydrogen charging was found to reduce the performance, as well as the thickness and oxide content of the passive films, mainly due to the capture of oxide atoms during strong oxidation of hydrogen atoms.

Dual‐Atom Catalysts Derived from a Preorganized Covalent Organic Framework for Enhanced Electrochemical Oxygen Reduction

AbstractDual‐atom catalysts (DAC) are deemed as promising electrocatalysts due to the abundant active sites and adjustable electronic structure, but the fabrication of well‐defined DAC is still full of challenges. Herein, bonded Fe dual‐atom catalysts (Fe2DAC) with Fe2N6C8O2 configuration were developed through one‐step carbonization of a preorganized covalent organic framework with bimetallic Fe chelation sites (Fe2COF). The transition from Fe2COF to Fe2DAC involved the dissociation of the nanoparticles and the capture of atoms by carbon defects. Benefitting from the optimized d‐band center and enhanced adsorption of OOH* intermediates, Fe2DAC exhibited outstanding oxygen reduction activity with a half‐wave potential of 0.898 V vs. RHE. This work will guide more fabrication of dual‐atom and even cluster catalysts from preorganized COF in the future.

Dual-Atom Catalysts Derived from a Preorganized Covalent Organic Framework for Enhanced Electrochemical Oxygen Reduction.

Dual-atom catalysts (DAC) are deemed as promising electrocatalysts due to the abundant active sites and adjustable electronic structure, but the fabrication of well-defined DAC is still full of challenges. Herein, bonded Fe dual-atom catalysts (Fe2DAC) with Fe2N6C8O2 configuration were developed through one-step carbonization of a preorganized covalent organic framework with bimetallic Fe chelation sites (Fe2COF). The transition from Fe2COF to Fe2DAC involved the dissociation of the nanoparticles and the capture of atoms by carbon defects. Benefitting from the optimized d-band center and enhanced adsorption of OOH* intermediates, Fe2DAC exhibited outstanding oxygen reduction activity with a half-wave potential of 0.898 V vs. RHE. This work will guide more fabrication of dual-atom and even cluster catalysts from preorganized COF in the future.

Influence of helium plasma on the structural state of the surface carbide layer of tungsten

<abstract> <p>This paper presents the results of the experimental studies of the helium plasma interaction with a surface carbide layer of tungsten. The experiments were carried out on a plasma beam installation (PBI) at a constant energy of incoming ions of 2 keV and at a surface temperature of the tungsten carbide layer of ~905 and ~1750 ℃. The local parameters (T<sub>e</sub>, n<sub>0</sub>) of the helium plasma were evaluated using the probe method and spectrometric analysis of the plasma composition. The helium plasma irradiated two types of the carbide layer on the tungsten surface, WC and W<sub>2</sub>C. The mechanisms of changing the tungsten surface morphology in the result of the plasma irradiation have been described. The study of the surface structure of the tungsten samples with a carbide layer of two types (WC, W<sub>2</sub>C) after the exposure to the helium plasma has revealed two different types of the formation of helium bubbles and changes in the surface morphology. The physical mechanism of the formation of helium bubbles consists in the capture of helium atoms by the thermal vacancies generated at high temperature by the material surface. However, with a significant increase in temperature to 1750 ℃, the formation of the bubbles was no longer observed and the sample surface had a developed coral-like structure with crystallographically oriented grains.</p> </abstract>

Mathematical model of solidification of melt with high-speed cooling

A new mathematical model of supercooled melt crystallization based on the variational principles of thermodynamics has been developed. The model takes into account the crystal formation and diffusion growth regularities, as well as the diffusionless crystal growth with the deviation from the local equilibrium at the surface. The model also takes into account the growing crystals mutual influence on the components concentration in the melt. The calculations for the supercooled eutectic melt Fe83B17 showed that the nucleation and growth of the phases Fe and Fe2B with a metastable phase Fe3B occur in the melt. The local equilibrium on the surface of the growing Fe3B crystals with the melt probably does not maintained. The regularities of the nucleation and mutual influence of the growing crystals of the phases are studied. The nucleation and growth rate of the Fe3B nuclei differs from the growth of Fe and Fe2B nuclei due to the diffusionless capture of boron atoms by the growing Fe3B crystals surface. The model will help to calculate the melt cooling technology mode for producing amorphous ribbons on a copper rotating drum. The calculation made it possible to analyze changes in the temperature and the crystallization degree in the various ribbon layers. The calculation results have been verified experimentally by x-ray diffraction and calorimetric studies of the obtained ribbons. The correspondence of the calculation and the experimental results confirms the effectiveness developed methodology for studying the regularities of crystal growth in supercooled melts.

Boron‐Tethering and Regulative Electronic States Around Iridium Species for Hydrogen Evolution

AbstractThe performance of single‐atom electrocatalysts usually suffers from attenuation due to high energy states, especially in harsh environments. Therefore, as high‐efficiency electrocatalysts for hydrogen reduction reaction (HER), supported metal nanoclusters (NCs) with maximum metal atom efficiency are promising, yet the genuine mechanism involving rational orbital modulation is still arguable. Herein, the conjugating effect between electron‐donor boron (B)‐tethering engineering and iridium (Ir) that facilitates the electron capture of Ir atoms is explored, achieving highly dispersive Ir‐NCs confined in N, B co‐doped defective carbon (Ir@NBD‐C). The Ir@NBD‐C catalyst achieves displays remarkable high activity for HER in a pH‐universal range, in particular, with an ultralow overpotential of 7 mV (10 mA cm−2), high mass activity of 652.2 A , and turnover frequency (TOF) of 1.90 H2 S−1 (100 mV) in 1.0 m KOH, outperforming almost all state‐of‐the‐art HER electrocatalysts. Operando characterizations and theoretical calculations unveil that the outstanding catalytic activity can attribute to the optimal binding to hydrogen intermediate species (H*) derived from the tunable and favorable electronic structure of the Ir site through the tethering of B heteroatoms. Undoubtedly, this work brings new insight into the design of catalysts with high intrinsic activity and thermodynamic stability.

Multiple bottle beams based on metasurface optical field modulation and their capture of multiple atoms

Compared to conventional devices, metasurfaces offer the advantages of being lightweight, with planarization and tuning flexibility. This provides a new way to integrate and miniaturize optical systems. In this paper, a metasurface capable of generating multiple bottle beams was designed. Based on the Pancharatnam–Berry (P–B) phase principle, the metasurface lens can accurately control the wavefront by adjusting the aspect ratio of the titanium dioxide nanopillars and the rotation angle. When irradiated by left-handed circularly polarized light with a wavelength of 632.8 nm, the optical system can produce multiple micron bottle beams. Taking two bottle beams as examples, the longitudinal full widths at half-maximum of the optical tweezers can reach 0.85 μm and 1.12 μm, respectively, and the transverse full widths at half-maximum can reach 0.46 μm and 0.6 μm. Also, the number of generated bottle beams can be varied by controlling the size of the annular obstacle. By changing the x-component of the unit rotation angle, the metasurface can also change the shape of the bottle beam — the beam cross-section can be changed from circular to elliptical. This paper also analyzes the trapping of ytterbium atoms by the multi bottle beam acting as optical tweezers. It is found that the multi bottle beam can cool and trap multiple ytterbium atoms.

The antinucleus annihilation reconstruction algorithm of the GAPS experiment

The General AntiParticle Spectrometer (GAPS) is an Antarctic balloon-borne detector designed to measure low-energy cosmic antinuclei (<0.25GeV/n), with a specific focus on antideuterons, as a distinctive signal from dark matter annihilation or decay in the Galactic halo. The instrument consists of a tracker, made up of ten planes of lithium-drifted Silicon Si(Li) detectors, surrounded by a plastic scintillator Time-of-Flight system. GAPS uses a novel particle identification method based on exotic atom capture and decay with the emission of pions, protons, and atomic X-rays from a common annihilation vertex.An important ingredient for the antinuclei identification is the reconstruction of the “annihilation star” topology. A custom antinucleus annihilation reconstruction algorithm, called the “star-finding” algorithm, was developed to reconstruct the annihilation star fully, determining the annihilation vertex position and reconstructing the tracks of the primary and secondary charged particles. The reconstruction algorithm and its performances were studied on simulated data obtained with the Geant4-based GAPS simulation software, which fully reproduced the detector geometry. This custom algorithm was found to have better performance in the vertex resolution and reconstruction efficiency compared with a standard Hough-3D algorithm.