Tailoring local structures of atomically dispersed copper sites for highly selective CO_(2) electroreduction

Atomically‐dispersed copper sites coordinated with nitrogen‐doped carbon(Cu–N–C)can provide novel possibilities to enable highly selective and active electrochemical CO_(2) reduction reactions.However,the construction of optimal local electronic structures for nitrogen‐coordinated Cu sites(Cu–N_(4))on carbon remains challenging.Here,we synthesized the Cu–N–C catalysts with atomically‐dispersed edge‐hosted Cu–N_(4) sites(Cu–N_(4)C_(8))located in a micropore between two graphitic sheets via a facile method to control the concentration of metal precursor.Edge‐hosted Cu–N_(4)C_(8) catalysts outperformed the previously reported M–N–C catalysts for CO_(2)‐to‐CO conversion,achieving a maximum CO Faradaic efficiency(FECO)of 96%,a CO current density of–8.97 mA cm^(–2) at–0.8 V versus reversible hydrogen electrode(RHE),and over FECO of 90%from–0.6 to–1.0 V versus RHE.Computational studies revealed that the micropore of the graphitic layer in edge‐hosted Cu–N_(4)C_(8) sites causes the d‐orbital energy level of the Cu atom to shift upward,which in return decreases the occupancy of antibonding states in the*COOH binding.This research suggests new insights into tailoring the locally coordinated structure of the electrocatalyst at the atomic scale to achieve highly selective electrocatalytic reactions.

Ultrafine ordered L1_(2)-Pt-Co-Mn ternary intermetallic nanoparticles as high-performance oxygen-reduction electrocatalysts for practical fuel cells

The long-range periodically ordered atomic structures in intermetallic nanoparticles(INPs)can significantly enhance both the electrocatalytic activity and electrochemical stability toward the oxygen reduction reaction(ORR)compared to the disordered atomic structures in ordinary solid-solution alloy NPs.Accordingly,through a facile and scalable synthetic method,a series of carbon-supported ultrafine Pt_3Co_(x)Mn_(1-x)ternary INPs are prepared in this work,which possess the"skin-like"ultrathin Pt shells,the ordered L1_(2) atomic structure,and the high-even dispersion on supports(L1_(2)-Pt_3Co_(x)Mn_(1-x)/~SPt INPs/C).Electrochemical results present that the composition-optimized L1_(2)-Pt_3Co_(0.7)Mn_(0.3)/~SPt INPs/C exhibits the highest electrocata lytic activity among the series,which are also much better than those of the pristine ultrafine Pt/C.Besides,it also has a greatly enhanced electrochemical stability.In addition,the effects of annealing temperature and time are further investigated.More importantly,such superior ORR electrocatalytic performance of L1_(2)-Pt_3Co_(0.7)Mn_(0.3)/~SPt INPs/C are also well demonstrated in practical fuel cells.Physicochemical characterization analyses further reveal the major origins of the greatly enhanced ORR electrocata lytic performance:the Pt-Co-Mn alloy-induced geometric and ligand effects as well as the extremely high L1_(2) atomic-ordering degree.This work not only successfully develops a highly active and stable ordered ternary intermetallic ORR electrocatalyst,but also elucidates the corresponding"structure-function"relationship,which can be further applied in designing other intermetallic(electro)catalysts.

Recent progress in two-dimensional metallenes and their potential application as electrocatalyst

In this article,we looked at metallenes,a novel class of two-dimensional(2D)metals that are attracting interest in the energy and catalysis sectors.Catalysis is one area where their exceptional physicochemical and electrical characteristics might be useful.Metallenes are unique because they include several metal atoms that are not in a coordinated bond.This makes them more active and improves their atomic uti-lization,which in turn increases their catalytic potential.This article delves into the potential of two-dimensional metals as electrocatalysts for carbon dioxide reduction,fuel oxidation,oxygen evolution,and oxygen reduction reactions in the context of sustainable energy conversion.Owing to the exception-ally high surface-to-volume ratio,large surface area as well as their optimized atomic use efficiency,2D materials defined by atomic layers are crucial for surface-related sustainable energy applications.Due to its exceptional properties,such as high conductivity and the ability to enhance the exposure of active metal sites,2D metallenes have recently attracted a lot of interest for use in catalysis,electronics,and energy-related applications.With their highly mobility,adjustable surface states,and electrical struc-tures that can be fine-tuned,2D metallenes are promising nanostructure materials for use in energy con-version with the sustainable applications.

Oxygen redox chemistry in lithium-rich cathode materials for Li-ion batteries:Understanding from atomic structure to nano-engineering

Lithium-rich oxide compounds have been recognized as promising cathode materials for high performance Li-ion batteries,owing to their high specific capacity.However,it remains a great challenge to achieve the fully reversible anionic redox reactions to realize high capacity,high stability,and low voltage hysteresis for lithiumrich cathode materials.Therefore,it is critically important to comprehensively understand and control the anionic redox chemistry of lithium-rich cathode materials,including atomic structure design,and nano-scale materials engineering technologies.Herein,we summarize the recent research progress of lithium-rich cathode materials with a focus on redox chemistry.Particularly,we highlight the oxygen-based redox reactions in lithium-rich metal oxides,with critical views of designing next generation oxygen redox lithium cathode materials.Furthermore,we purposed the most promising strategies for improving the performances of lithium-rich cathode materials with a technology-spectrum from the atomic scale to nano-scale.

Atomic structure and collision dynamics with highly charged ions

The research progresses on the investigations of atomic structure and collision dynamics with highly charged ions based on the heavy ion storage rings and electron ion beam traps in recent 20 years are reviewed.The structure part covers test of quantum electrodynamics and electron correlation in strong Coulomb field studied through dielectronic recombi-nation spectroscopy and VUV/x-ray spectroscopy.The collision dynamics part includes charge exchange dynamics in ion-atom collisions mainly in Bohr velocity region,ion-induced fragmentation mechanisms of molecules,hydrogen-bound and van de Waals bound clusters,interference,and phase information observed in ion-atom/molecule collisions.With this achievements,two aspects of theoretical studies related to low energy and relativistic energy collisions are presented.The applications of data relevant to key atomic processes like dielectronic recombination and charge exchanges involving highly charged ions are discussed.At the end of this review,some future prospects of research related to highly charged ions are proposed.

Atomic structure and transition properties of H-like Al in hot and dense plasmas

The atomic structure and transition properties of H-like Al embedded in hot and dense plasmas are investigated using modified GRASP2 K code. The plasma screening effect on the nucleus is described using the self-consistent field ion sphere model. The effective nuclear potential decreases much more quickly with increasing average free electron density,but increases slightly with increasing electron temperature. The variations of the transition energies, transition probabilities,and oscillator strengths with the free electron density and electron temperature are the same as that of the effective nuclear potential. The results reported in this work agree well with other available theoretical results and are useful for plasma diagnostics.

A New Theory on the Origin and Nature of the Fine Structure Constant

The nature and the origin of the fine structure are described. Based on the vortex model and hydrodynamics, a comprehensible interpretation of the fine structure constant is developed. The vacuum considered to have superfluid characteristics and elementary particles such as the electron and Hydrogen molecule are irrotational vortices of this superfluid. In such a vortex, the angular rotation ω is maintained, and the larger the radius, the slower the rotational speed. The fine structure value is derived from the ratio of the rotational speed of the boundaries of the vortex to the speed of the vortex eye in its center. Since the angular rotation is constant, the same value was derived from the ratio between the radius of the constant vortex core and the radius of the hall vortex. Therefore, the constancy of alpha is an expression of the constancy relation in the vortex structure.

Molecular Dynamics Study on Interfacial Energy and Atomic Structure of Ag/Ni and Cu/Ni Heterophase System

The results of molecular dynamics calculations on the interfacial energies and atomic structures of Ag/Ni and Cu/Ni interfaces are presented. Calculation on Ag/Ni interfaces with low-index planes shows that those containing the (111) plane have the lowest energies, which is in agreement with the experiments. Comparing surface energy with interfacial energy, it is found the order of the interfacial energies of Ag/Ni and Cu/Ni containing the planes fall in the same order as solid-vapor surface energies of Ag, Cu and Ni. In this MD simulation, the relaxed atomic structure and dislocation network of (110)_Ag||(110)Ni interface are coincident to HREM observations.

Investigations about the Atomic Structure and Mechanical Behavior of Metallic Glasses after Melt Hydrogenation

“Hydrogen in metallic glasses”has become a popular topic for material scientists,yet few studies focus on the atomic⁃scale details.Herein,by utilizing molecular dynamic simulations,the changes on the atomic structure of Cu50Zr50 metallic glasses after melt hydrogenation were systematically analyzed,with the aim of understanding the differences of mechanical behavior between these amorphous alloys.The simulated analyses indicate that the hydrogenated samples become more compact than the H⁃free one,but the fraction of the dominant coordination polyhedra with higher degree of local fivefold symmetry significantly decreases accompanied by the addition of H atoms.Accordingly,melt hydrogenation can induce much more local“soft spots”in metallic glasses to alleviate the degree of strain localization during deformation,i.e.,it has a positive influence on the deformability of glassy alloys in agreement with experimental results.

Quasilattice-Conserved Optimization of the Atomic Structure of Decagonal Al-Co-Ni Quasicrystals

The detailed atomic structure of quasicrystals has been an open problem for decades. Here we present a quasilattiee-conserved optimization method （quasi-OPT）, under particular quasiperiodic boundary conditions. As the atomic coordinates are described by basic cells and quasilattices, we are able to maintain the self-similarity characteristics of qusicrystals with the atomic structure of the boundary region updated timely following the relaxing region. Exemplified with the study of decagonal Al-Co-Ni （d-Al-Co-Ni）, we propose a more stable atomic structure model based on Penrose quasilattice and our quasi-OPT simulations. In particular, rectangle-triangle ruIes are suggested for the local atomic structures of d-Al-Co-Ni quasicrystals.

Studies of Atomic Structure and Physical Properties of Metal Clusters in MgO by HREM and Nano-probe Methods

Nanometer-sized metal clusters were prepared inside single crystalline MgO films by vacuum co-deposition of metals and MgO. The atomic structure was studied by high-resolution electron microscopy (HREM) and nm-area electron diffraction. The size of the clusters is ranging from 1 nm to 3 nm without those larger than 5 nm, and most of them have definite epitaxial orientations with the MgO matrix films. The character of the composite films is very much useful for the studies of various kinds of physical properties with anisotroPy. The physical properties such as electric transport, magnetic, optical absorption, sintering and catalytic ones were thus measured on the same samples analyzed by HREM by using high sensitivity apparatus with interest of clarifying the retationship between the atomic structure and physical properties

Velocity-selective spectroscopy measurements of Rydberg fine structure states in a hot vapor cell

A velocity-selective spectroscopy technique for studying the spectra of Rydberg gases is presented. This method provides high-resolution spectrum measurements. We present experimental results for a ladder system 6S1/2→ 6P3/2→ nS（D）electromagnetically-induced transparency involving highly-excited Rydberg states. Based on a radio-frequency modulation technique, we measure the hyperfine structure splitting of intermediate states and the fine structure splitting of Rydberg states in a room temperature ^133Cs vapor cell. The experimental data and theoretical predictions show excellent agreement.

Molecular Structure of Atomic Nucleus

In this work, we extend our work on the Heisenberg model of the neutron formulated as a dwarf hydrogen-like atom under the influence of the More General Exponential Screened Coulomb Potential (MGESCP) to show that an atomic nucleus may possess a molecular structure made up of atoms bonding together by a potential used to describe the strong force associated with a generalised Yukawa MGESCP potential. We show that the neutrons and protons are arranged into narrow lattices therefore they may fold to form three-dimensional shells by bonding similar to hydrogen bonding. In particular, the nucleons may form stable structures such as that of fullerenes in which the vertices are occupied by the nucleons which are simply just protons. For example, a nucleus with a total number of 60 nucleons may arrange itself into the topological structure of a buckminsterfullerene. We also apply Schrödinger wave equation with central field approximation to describe the quantum dynamics of nuclei of atomic atoms that now possess the physical structure of a dwarf molecular ion.

A Generic Description Model for the Structure of Atomic Nucleus with New Interpretation of the Strong Forces

The present investigation is motivated by finding and developing an easily understandable solution in the context of unified quantum and gravitational theories. Model-based methods are applied, with emphasis on structural descriptions by introducing some strong hypotheses. A subset of the introduced hypotheses led to a surprising understanding of the internal structure and construction of quarks, neutrons, protons and more complex atomic nuclei. The research work therefore focused mainly on the model-based interpretation of subatomic processes. The results obtained so far and presented in this paper are new. They consist of a generic description model for the structure of atomic nuclei. This model contains two important structural links that originate from the initial phase of the cosmological big bang. They hold atomic parts together and are involved in many known nuclear fusion and fission processes. Modifications of them, including the electron-positron annihilation process, are necessary and will be described. A new interpretation of the strong forces from the Standard Model is possible and will be given. In addition, the formation processes for electron and positron particles are considered. Based on the structural relationships, a deeper understanding of matter transformations (transmutations), early cosmological processes and dark matter has been achieved. All challenges of this work are the logical conclusions from the used hypotheses on two structural links. They need to be further investigated and verified by theoretical and experimental works. The postulated particle in this paper, as accompanying product in the electron-positron annihilation, will play a major role for the future investigations.

Diverse atomic structure configurations of metal-doped transition metal dichalcogenides for enhancing hydrogen evolution

Doping foreign metal atoms into the substrate of transition metal dichalcogenides(TMDs)enables the formation of diverse atomic structure configurations,including isolated atoms,chains,and clusters.Therefore,it is very important to reasonably control the atomic structure and determine the structure-activity relationship between the atomic configurations and the hydrogen evolution reaction(HER)performance.Although numerous studies have indicated that doping can yield diverse atomic structure configurations,there remains an incomplete understanding of the relationship between atomic configurations within the lattice of TMDs and their performance.Here,diverse atomic structure configurations of adsorptive doping,substitutional doping,and TMDs alloys are summarized.The structure-activity relationship between different atomic configurations and HER performance can be determined by micro-nanostructure devices and density functional theory(DFT)calculations.These diverse atomic structure configurations are of great significance for activating the inert basal plane of TMDs and improving the catalytic activity of HER.Finally,we have summarized the current challenges and future opportunities,offering new perspectives for the design of highly active and stable metal-doped TMDs catalysts.

Asymmetric N,O-Coordinated Single Atomic Co Sites for Stable Lithium Metal Anodes

Lithium metal has been considered one of the most promising anodes for next-generation rechargeable batteries,but its practical application is largely hindered by the uncontrollable dendrite growth and infinite volume change.Here,inspired by superior catalytic effects of single-atom catalysts,carbon-supported single atomic Co with asymmetric N,O-coordination(Co-N/O)is developed for Li metal battery.Experimental results and theoretical calculations indicate that single atomic Co atoms with asymmetric N,O-coordination present enhanced binding ability toward Li in comparison with N-coordinated atomic Co site and isolated O site,enabling uniform Li plating/stripping.Moreover,the asymmetric N,O-coordination around Co atoms induces co-activation effects,lowering the energy barriers toward Li^(+)to Li^(0)conversion and largely promoting the deposition kinetics.When used as a Li deposition host,the Co-N/O achieves a high average coulombic efficiency of 98.6%at a current density of 1 mA cm^(-2)and a capacity of 2 mAh cm^(-2),long cycling life of 2000 h in symmetrical cells,and excellent rate performance(voltage hysteresis of 23 mV at 8 mA cm^(-2)).This work provides a comprehensive understanding of single atomic metals with asymmetric heteroatom coordination in the design of Li metal anode.

Ab initio study of chemical effect on structural properties of Ti–Al melts

We study chemical effect on the structural properties of Ti–Al melts, with the Al concentration systematically changed,via ab initio molecular dynamics simulations. By calculating the partial coordination numbers, we find a preferred connection between the nearest neighbors for Al–Ti pairs. This induces an excess Ti coordination in the cluster characterized by local five-fold symmetry in Voronoi tessellation. Structural entropy measured from the diversity of Voronoi polyhedrons shows an intriguing non-monotonic tendency with concentration: it first decreases to a minimum value at Ti_(40)Al_(60), and then increases beyond this concentration. This implies a more ordered local structure induced by the chemical interaction at the intermediate compositions. The spatial correlation among the crystalline-like or the icosahedral-like clusters also exhibits the highest intensity for Al–Ti pairs, verifying the important role played by the chemical interaction in the local structure connectivity.

Interplay between the atomic structures and superconductivity of two-monolayer Pb films

Superconductors with reduced dimensionality have been widely explored for their exotic superconducting behaviors.Especially,at the two-dimensional limit,two-monolayer Pb films with two types of structures provide an ideal platform to unveil the underlying superconducting mechanism[Science 324,1314(2009)].Here,by combining scanning tunneling microscopy(STM)with the first-principle calculations,we successfully identify that these two types have different atomic lattice structures with varying stacking phases,which further enables us to calculate the phonon spectrum and electron phonon coupling strength of each type.The theoretical calculations are in good agreement with tunneling spectroscopy measurements of the superconducting transition temperatures(T_(c)),which established a correlation between atomic structures and superconductivity.Moreover,it was observed that the higher T_(c)of these two types also possess higher out-of-plane upper critical magnetic fields(Hc2).These findings will provide important new insights into two-dimensional superconductivity at the atomic level.

MicroED as a powerful technique for the structure determination of complex porous materials

Porous materials have garnered significant attention in recent years.Understanding the intrinsic relationship between their structures and properties requires precise knowledge of their atomic structures.Single-crystal X-ray diffraction(SCXRD)has traditionally been the primary method for elucidating such structures,but it demands large,high-quality crystals,often exceeding 5μm in size.The growth of these crystals can be a time-consuming process,especially for one-and two-dimensional materials.To explore structures at the nanoscale,MicroED(microcrystal electron diffraction(ED))offers unprecedented insights into the realm of nanomaterials.This revolutionary technique enables researchers to uncover intricate details within nanoscale structures,promising to reshape our fundamental understanding of materials.In this review,we delve into the applications of MicroED in the study of various porous materials,including zeolites,metal-organic frameworks(MOFs),and covalent organic frameworks(COFs).We emphasize the pivotal role of MicroED in nanomaterial characterization,enabling precise crystallographic analysis and phase identification.

Study on Modification Mechanism of Rare Earth in ZA27 Cast Alloy with Electronic Theory and Molecular Dynamics Method

A model of liquid ZA27 cast alloy is established according to molecular dynamics theory and an atomic structural model of co-existent a phase and liquid is also presented by means of computer programming. Recursion method is adopted to calculate the electronic structure of RE (rare earth) in grains and around phase boundaries respectively. The calculation shows that RE is more stable around phase boundaries than in grains, which explains the fact that the solution of RE in a phase is less, and RE mainly aggregates in front of phase boundary. The calculations of bonding order integrals also show that RE in front of phases hardly solidify onto the grain surfaces as active element so as to prevent grains growth and refine the grains. As a result, the modification mechanism of RE may be explained from the view of electronic structure.