Single Atomic Vacancy Catalysis.

Single atom catalysts provide exceptional activity. However, measuring the intrinsic catalytic activity of a single atom in real electrochemical environments is challenging. Here, we report the activity of a single vacancy for electrocatalytically evolving hydrogen in two-dimensional (2D) MoS.

Identification of Non-Carbonaceous Cathodes in Al Batteries: Potential Applicability of Black and Blue Phosphorene Monolayers.

In the present era of growing energy demands, low-dimensional materials are emerging as the suitable choices for energy storage due to their excellent ion transport properties, improved reversible capacity, fine rate performance and good cycling stability. In this context, we have investigated the applicability of black and blue phosphorene monolayers as potential cathodes for Al batteries. Both black and blue phosphorene monolayers show similar electrochemical behavior as that of experimentally reported graphite with a charge transfer from the surface in order to bind the tetrahedral geometry of AlCl during the charging process.

Guest-Induced Ultrasensitive Detection of Multiple Toxic Organics and Fe Ions in a Strategically Designed and Regenerative Smart Fluorescent Metal-Organic Framework.

Luminescent metal-organic frameworks (LMOFs) are promising functional materials for sustainable applications, where an analyte-induced multiresponsive system with good recyclability is beneficial for detecting numerous lethal pollutants. We designed and built the dual-functionalized, three-dimensional Zn(II)-framework [Zn( bpg)( azdc)]·(DMF)·(HO) (CSMCRI-1) using an -OH group-integrated bpg linker and a -N═N- moiety containing H azdc ligand, which functions as a unique tetrasensoric fluorescent probe. The activated CSMCRI-1 (1') represents the hitherto unreported pillar-layer framework for extremely selective fluorescence quenching by nitrofurazone antibiotics as well as explosive nitro-aromatic 2,4,6-trinitrophenol, where ultrasensitive detection is achieved for both the electron-lacking analytes.

Strain-mediated effects of oxygen deficiency and variation in non-Fermi liquid behavior of epitaxial PrNiO thin films.

To understand the effects of oxygen variation in combination with different strains in perovskite nickelates, three sets of PrNiO thin films S , S and S were deposited on (0 0 1) oriented single-crystal wafers of SrTiO, LSAT [(LaAlO)(SrTaAlO)] and LaAlO, respectively. Two sets of films, S and S , have tensile strain whereas the films of S show compressive strain. For each set, two thin films of fixed thickness (5 nm) were deposited; one film was annealed in situ in oxygen partial pressure just after deposition, the other film was not annealed.

Role of Dimensionality for Photocatalytic Water Splitting: CdS Nanotube versus Bulk Structure.

Using state-of-the-art density functional theoretical calculations, we have modelled a facetted CdS nanotube (NT) catalyst for photocatalytic water splitting. The overall photocatalytic activity of the CdS photocatalyst has been predicted based on the electronic structures, band edge alignment, and overpotential calculations. For comparisons, we have also investigated the water splitting process over bulk CdS.

Ferromagnetism in magnesium chloride monolayer with an unusually large spin-up gap.

The primary research target of the rapidly evolving spintronic industry is to design highly efficient novel materials that consume very low power and operate with high speed. Main group based ferromagnetic half-metallic materials are very promising due to their long spin-relaxation time. In recent years, the discovery of superconducting state with high critical temperature in a magnesium based system (MgB) invigorated researchers due to its simple crystal structure and intriguing results, leading to its use as a good material for large scale application in electronic devices.

High-energy-density dual-ion battery for stationary storage of electricity using concentrated potassium fluorosulfonylimide.

Graphite dual-ion batteries represent a potential battery concept for large-scale stationary storage of electricity, especially when constructed free of lithium and other chemical elements with limited natural reserves. Owing to their non-rocking-chair operation mechanism, however, the practical deployment of graphite dual-ion batteries is inherently limited by the need for large quantities of electrolyte solutions as reservoirs of all ions that are needed for complete charge and discharge of the electrodes. Thus far, lithium-free graphite dual-ion batteries have employed moderately concentrated electrolyte solutions (0.

High Curie temperature and half-metallicity in an atomically thin main group-based boron phosphide system: long range ferromagnetism.

Transition metal-free magnetism and half-metallicity are currently drawing remarkable attention due to their potential future applications in spintronics devices. Using state-of-the-art density functional theory (DFT) calculations, we have considered Be and Mg incorporated in atomically thin boron phosphide (BP) systems for possible spintronics applications. Interestingly, our results reveal that Mg and Be substitution at P-sites exhibits ferromagnetism and half-metallicity.

Correlation of structure with UV-visible spectra by varying SH composition in Au-SH nanoclusters.

In the present work, we model artificial neural network (ANN) potentials for Au (SH) nanoclusters in the range of = 10 to = 38. The accuracy of ANN potentials is tested by comparing the global minimum (GM) structures of Au (SH) nanoclusters, at saturated amount of SH, with the earlier reported structures. The GM structures are reported for the first time for nanoclusters with compositions lower than the saturated SH composition.

First-Principles Study of Magnesium Peroxide Nucleation for Mg-Air Battery.

Recently, rechargeable non-aqueous Mg-air batteries have gained a lot of interest as the next-generation energy storage device due to the high theoretical volumetric density (3832 Ah L for Mg anode vs. 2062 Ah L for Li), low cost and safety. The field of Mg-air batteries is in the initial stage of development having a limited number of experimental and theoretical reports, in which mainly a carbon cathode is used; however, the information regarding the structural form of carbon is still missing.

Phytochemicals as modulators of M1-M2 macrophages in inflammation.

Macrophages are critical mediators of the innate immune response against foreign pathogens, including bacteria, physical stress, and injury. Therefore, these cells play a key role in the "inflammatory pathway" which in turn can lead to an array of diseases and disorders such as autoimmune neuropathies and myocarditis, inflammatory bowel disease, atherosclerosis, sepsis, arthritis, diabetes, and angiogenesis. Recently, more studies have focused on the macrophages inflammatory diseases since the discovery of the two subtypes of macrophages, which are differentiated on the basis of their phenotype and distinct gene expression pattern.

Investigation of Dual-Ion Beam Sputter-Instigated Plasmon Generation in TCOs: A Case Study of GZO.

The use of the high free-electron concentration in heavily doped semiconductor enables the realization of plasmons. We report a novel approach to generate plasmons in Ga:ZnO (GZO) thin films in the wide spectral range of ∼1.87-10.

Stanene based gas sensors: effect of spin-orbit coupling.

Density functional theory calculations are performed to investigate the gas sensing properties (NO, NO, NH and NO) of pure and doped (B@, N@, and B-N@) stanene. Dispersion corrected (DFT-D3) density functional calculations show that doping improves the interaction between stanene and gas molecules. The extent of interaction between the system and gas molecules is further studied through charge density difference (CDD), electrostatic potential (ESP) and Bader charge analysis.

c-T phase diagram and Landau free energies of (AgAu) nanoalloy via neural-network molecular dynamic simulations.

For understanding the structure, dynamics, and thermal stability of (AgAu) nanoalloys, knowledge of the composition-temperature (c-T) phase diagram is essential due to the explicit dependence of properties on composition and temperature. Experimentally, generating the phase diagrams is very challenging, and therefore theoretical insight is necessary. We use an artificial neural network potential for (AgAu) nanoalloys.

Ferromagnetism and Half-Metallicity in a High-Band-Gap Hexagonal Boron Nitride System.

Metal-free half-metallicity is the subject of intense research in the field of spintronics devices. Using density functional theoretical calculations, atom-thin hexagonal boron nitride (h-BN)-based systems are studied for possible spintronics applications. Ferromagnetism is observed in patterned C-doped h-BN systems.

Ferromagnetism and Half-Metallicity in Atomically Thin Holey Nitrogenated Graphene Based Systems.

Metal-free half-metallicity has been the subject of immense research focus in the field of spintronic devices. By using density functional theoretical (DFT) calculations, atomically thin holey nitrogenated graphene (C N) based systems are studied for possible spintronic applications. Ferromagnetism is observed in all the C-doped holey nitrogenated graphene.

Bimetallic core-based cuboctahedral core-shell nanoclusters for the formation of hydrogen peroxide (2e reduction) over water (4e reduction): role of core metals.

The design of an efficient and selective catalyst for hydrogen peroxide (HO) formation is highly sought due to its industrial importance. As alternatives to a conventional Pd-Au alloy-based catalyst, three cuboctahedral core-shell nanoclusters (Au@Pt, Co@Pt and AuCo@Pt NCs) have been investigated. Their catalytic activities toward HO formation have been compared with that of pure Pt cuboctahedral NC (Pt).

A Computational Study of a Single-Walled Carbon-Nanotube-Based Ultrafast High-Capacity Aluminum Battery.

Exploring suitable electrode materials is a fundamental step toward developing Al batteries with enhanced performance. In this work, we explore using density functional theory calculations the feasibility of single-walled carbon nanotubes (SWNTs) as a cathode material for Al batteries. Carbon nanotubes with hollow structures and large surface area are able to overcome the difficulty of activating the opening of interlayer spaces as observed in graphite electrode during the first intercalation cycle.

The staging mechanism of AlCl intercalation in a graphite electrode for an aluminium-ion battery.

Identifying a suitable electrode material with desirable electrochemical properties remains a primary challenge for rechargeable Al-ion batteries. Recently an ultrafast rechargeable Al-ion battery was reported with high charge/discharge rate, (relatively) high discharge voltage and high capacity that uses a graphite-based cathode. Using calculations from first-principles, we have investigated the staging mechanism of AlCl intercalation into bulk graphite and evaluated the stability, specific capacity and voltage profile of AlCl intercalated compounds.

Neural network potentials for dynamics and thermodynamics of gold nanoparticles.

For understanding the dynamical and thermodynamical properties of metal nanoparticles, one has to go beyond static and structural predictions of a nanoparticle. Accurate description of dynamical properties may be computationally intensive depending on the size of nanoparticle. Herein, we demonstrate the use of atomistic neural network potentials, obtained by fitting quantum mechanical data, for extensive molecular dynamics simulations of gold nanoparticles.

Interplay among Electrostatic, Dispersion, and Steric Interactions: Spectroscopy and Quantum Chemical Calculations of π-Hydrogen Bonded Complexes.

π-Hydrogen bonding interactions are ubiquitous in both materials and biology. Despite their relatively weak nature, great progress has been made in their investigation by experimental and theoretical methods, but this becomes significantly more complicated when secondary intermolecular interactions are present. In this study, the effect of successive methyl substitution on the supramolecular structure and interaction energy of indole⋅⋅⋅methylated benzene (ind⋅⋅⋅n-mb, n=1-6) complexes is probed through a combination of supersonic jet experiments and benchmark-quality quantum chemical calculations.

Protection of Endogenous Thiols against Methylmercury with Benzimidazole-Based Thione by Unusual Ligand-Exchange Reactions.

Organomercurials, such as methylmercury (MeHg ), are among the most toxic materials to humans. Apart from inhibiting proteins, MeHg exerts its cytotoxicity through strong binding with endogenous thiols cysteine (CysH) and glutathione (GSH) to form MeHgCys and MeHgSG complexes. Herein, it is reported that the N,N-disubstituted benzimidazole-based thione 1 containing a N-CH CH OH substituent converts MeHgCys and MeHgSG complexes to less toxic water-soluble HgS nanoparticles (NPs) and releases the corresponding free thiols CysH and GSH from MeHgCys and MeHgSG, respectively, in solution by unusual ligand-exchange reactions in phosphate buffer at 37 °C.

Band gap opening in stanene induced by patterned B-N doping.

Stanene is a quantum spin Hall insulator and a promising material for electronic and optoelectronic devices. Density functional theory (DFT) calculations are performed to study the band gap opening in stanene by elemental mono-doping (B, N) and co-doping (B-N). Different patterned B-N co-doping is studied to change the electronic properties of stanene.

C-H Bond Activation/Arylation Catalyzed by Arene-Ruthenium-Aniline Complexes in Water.

Water-soluble arene-ruthenium complexes coordinated with readily available aniline-based ligands were successfully employed as highly active catalysts in the C-H bond activation and arylation of 2-phenylpyridine with aryl halides in water. A variety of (hetero)aryl halides were also used for the ortho-C-H bond arylation of 2-phenylpyridine to afford the corresponding ortho- monoarylated products as major products in moderate to good yields. Our investigations, including time-scaled NMR spectroscopy and mass spectrometry studies, evidenced that the coordinating aniline-based ligands, having varying electronic and steric properties, had a significant influence on the catalytic activity of the resulting arene-ruthenium-aniline-based complexes.

Transition-metal embedded carbon nitride monolayers: high-temperature ferromagnetism and half-metallicity.

High-temperature ferromagnetic materials with planar surfaces are promising candidates for spintronics applications. Using state-of-the-art density functional theory (DFT) calculations, transition metal (TM = Cr, Mn, and Fe) incorporated graphitic carbon nitride (TM@gt-C3N4) systems are investigated as possible spintronics devices. Interestingly, ferromagnetism and half-metallicity were observed in all of the TM@gt-C3N4 systems.