Tip carbon encapsulation customizes cationic enrichment and valence stabilization for low K acidic CO electroreduction.

Acidic electrochemical CO conversion is a promising alternative to overcome the low CO utilization. However, over-reliance on highly concentrated K to inhibit the hydrogen evolution reaction also causes (bi)carbonate precipitation to interfere with catalytic performance. In this work, under the screening and guidance of computational simulations, we present a carbon coated tip-like InO electrocatalyst for stable and efficient acidic CO conversion to synthesize formic acid (HCOOH) with low K concentration.

Schottky Defects Suppress Nonradiative Recombination in CHNHPbI through Charge Localization.

Hybrid lead halide perovskites are promising materials for photovoltaic applications due to their exceptional optoelectronic properties. Here, we investigate the impact of Schottky defects─specifically PbI(V) and CHNHI (V) vacancies─on nonradiative recombination in CHNHPbI using time-dependent density functional theory and nonadiabatic (NA) molecular dynamics. Our results reveal that Schottky defects do not alter the fundamental bandgap or introduce trap states but instead distort the surrounding lattice, localizing the hole distribution.

Improving the Cycling Stability of NCM811 at High-Voltage 4.5V in Ester-Based Electrolytes with LiDFOB.

Nickel-rich layered cathode materials, particularly LiNiMnCoO (NCM811), have garnered significant attention due to their high energy density and impressive electrochemical performance. However, their cycling stability is compromised at elevated voltages, primarily due to structural instability and interfacial degradation. In this study, lithium difluoro(oxalato)borate (LiDFOB) is introduced into a commercial electrolyte based on lithium hexafluorophosphate (LiPF) to elucidate the structural and interfacial changes occurring in NCM811 at a high cut-off voltage of 4.

Dielectric Barrier Corona Activation of Electrical Discharge in a Cavitating Liquid.

Water treatment methods based on cold plasma discharge in cavitating liquid have been actively developing in recent years. However, some conditions, such as the conductivity of the medium, can limit the possibility of plasma ignition. The authors proposed a new method for activating an electric discharge in a cavitating liquid environment based on the use of an external corona discharge electrode in the plasma reactor.

Wave Function Localization Reduces the Bandgap of Disordered Double Perovskite CsAgBiBr.

Double perovskite CsAgBiBr is a promising alternative to lead-based perovskites with excellent stability and attractive optoelectronic properties. However, a relatively large bandgap severely limits its performance in many applications such as solar cells and photodetectors. It has been reported that a random distribution of Ag and Bi atoms in CsAgBiBr effectively reduces its bandgap without introducing dopants or impurities, while the mechanism remains unclear.

Dynamics of Vortex Matter in 2D Gapless Superconducting Materials with Impurities.

The recent interest in using ultrafast single-photon detectors in research and commercial applications has garnered significant attention from the scientific community. The dynamic event in the detection process consists of a photon causing local destruction of the order parameter, and then the applied current dissipates heat, bringing the material even more out of the superconducting state and then spiking a voltage peak in a measurement device. We investigated the role of superconducting and thermal parameters of the Generalized Time-Dependent Ginzburg-Landau (GTDGL) theory within the event of the first vortex penetration and the thermal dissipation in superconductors near the critical temperature.

The origin of broadband blue emission in zero-dimensional organic lead iodine perovskites: A first-principles study.

Broadband blue emission in zero-dimensional perovskites has received considerable attention, which is very important for the realization of stable blue-light emitters; however, the underlying formation mechanism remains unclear. Based on first-principles calculations, we have systematically studied the self-trapped excitons (STEs) behavior and luminescence properties in 0D-(DMA)4PbI6 perovskite. Our calculations show that there is a significant difference between the intrinsic STE luminescence mechanism (∼2.

Identifying Rare Events in Quantum Molecular Dynamics of Nanomaterials with Outlier Detection Indices.

Nanoscale and condensed matter systems evolve on multiple length- and time-scales, and rare events such as local phase transformation, ion segregation, defect migration, interface reconstruction, and grain boundary sliding can have a profound influence on material properties. We demonstrate how outlier detection indices can be used to identify rare events in machine-learning based, high-dimensional molecular dynamics (MD) simulations. Designed to order data-points from typical to untypical, the indices enable one to capture atomic events that are hard to detect otherwise.

Ab Initio Study of the Influence of Spin and Orbital Magnetic Moments on the Stability of Magnetic and Charge Distribution in Co:ZnO Monolayer.

The development of ultrathin magnets with tunable magnetic properties is essential for advancing quantum computing technologies. In this study, density functional theory (DFT) calculations were employed to investigate the atomic and electronic structures of a ZnO monolayer embedded with cobalt atoms. The impact of spin dynamics on charge transfer within the Co:ZnO system was thoroughly examined.

Formation and Recombination Dynamics of Polarons in Goethite: A Time-Domain Ab Initio Study.

The temperature and the coordination environment significantly affect polaron dynamics. Using goethite (FeOOH) as a model, our study examines polaron formation and recombination behavior under various conditions, including electron injection, photoexcitation, and heterovalent doping. Ab initio and nonadiabatic molecular dynamics (NAMD) simulations reveal that polaron formation in FeOOH is dependent on temperature via an adiabatic mechanism with higher temperatures leading to shorter formation times.

Breaking the size limitation of nonadiabatic molecular dynamics in condensed matter systems with local descriptor machine learning.

Nonadiabatic molecular dynamics (NA-MD) is a powerful tool to model far-from-equilibrium processes, such as photochemical reactions and charge transport. NA-MD application to condensed phase has drawn tremendous attention recently for development of next-generation energy and optoelectronic materials. Studies of condensed matter allow one to employ efficient computational tools, such as density functional theory (DFT) and classical path approximation (CPA).

Decoherence ensures convergence of non-adiabatic molecular dynamics with number of states.

Non-adiabatic (NA) molecular dynamics (MD) is a powerful approach for studying far-from-equilibrium quantum dynamics in photophysical and photochemical systems. Most NA-MD methods are developed and tested with few-state models, and their validity with complex systems involving many states is not well studied. By modeling intraband equilibration and interband recombination of charge carriers in MoS2, we investigate the convergence of three popular NA-MD algorithms, fewest switches surface hopping (FSSH), global flux surface hopping (GFSH), and decoherence induced surface hopping (DISH) with the number of states.

La(FeCuMnMgTi)O High-Entropy Oxide Nanoparticles as Highly Efficient Catalysts for Solvent-Free Aerobic Oxidation of Benzyl Alcohol.

In this work, a solid-state method for the synthesis of perovskite La(FeCuMnMgTi)O high-entropy oxide (HEO) nanoparticles is detailed. Additionally, the high performance of these nanoparticles as catalysts in the aerobic and solvent-free oxidation of benzyl alcohol is demonstrated. The structural features of HEO nanoparticles are studied by X-ray diffraction and high-resolution transmission electron microscopy.

Origin of the Improved Photoelectrochemical and Photocatalytic Activity in a ZnO-TiO Nanohybrid Revealed by Experimental and Density Functional Theory Studies.

Heterojunctions of metal oxides have attracted a great deal of attention as photo (electro) catalysts owing to their excellent photoactivity. While multiple fundamental studies have been dedicated to heteroaggregation, self-assembly of oppositely charged particles to obtain heterojunctions for energy applications has been underexplored. Herein, we report the synthesis of ZnO-TiO heterojunctions using the electrostatic self-assembly approach.

Quantum-confined bismuth iodide perovskite nanocrystals in mesoporous matrices.

Bismuth iodide perovskite nanocrystals are considered a viable alternative to the Pb halide ones due to their reduced toxicity and increased stability. However, it is still challenging to fabricate nanocrystals with a small and controlled size, and their electronic properties are not well understood. Here, we propose the growth of Bi iodide perovskite nanocrystals using different mesoporous silica with ordered pores of controlled diameter as templates.

High-Entropy La(FeCuMnMgTi)O Nanoparticles as Heterogeneous Catalyst for CO Electroreduction Reaction.

In this work, La(FeCuMnMgTi)O HEO nanoparticles with a perovskite-type structure are synthesized and used in the electrocatalytic CO reduction reaction (CORR). The catalyst demonstrates high performance as an electrocatalyst for the CORR, with a Faradaic efficiency (FE) of 92.5% at a current density of 21.

Compression Eliminates Charge Traps by Stabilizing Perovskite Grain Boundary Structures: An Ab Initio Analysis with Machine Learning Force Field.

Grain boundaries (GBs) play an important role in determining the optoelectronic properties of perovskites, requiring an atomistic understanding of the underlying mechanisms. Strain engineering has recently been employed in perovskite solar cells, providing a novel perspective on the role of perovskite GBs. Here, we theoretically investigate the impact of axial strain on the geometric and electronic properties of a common CsPbBr GB.

Ferroelectric Polarization and Single-Atom Catalyst Synergistically Promoting CO Photoreduction of CuBiPSe.

Further improving the activity and selectivity of photocatalytic CO reduction remains a challenge. Herein, we propose a new strategy for synergistically promoting photocatalytic CO reduction by combining two-dimensional (2D) ferroelectric polarization and single-atom catalysis. Our calculations showed that the ferroelectric polarization of CuBiPSe provides the internal driving force for the separation and migration of photogenerated carriers, which provides a prerequisite for enhancing the photocatalytic efficiency.

Improved Carrier Separation and Recombination by Ferroelectric Polarization in the CuBiPSe/CN Heterostructure: A Nonadiabatic Molecular Dynamics Study.

The rapid recombination of photogenerated carriers heavily restricts the photocatalytic efficiency. Here, we propose a new strategy to improve catalytic efficiency based on the ferroelectric van der Waals heterostructure (CuBiPSe/CN). Combining density functional theory and the nonadiabatic molecular dynamics (NAMD) method, we have systematically analyzed the ground-state properties and carrier dynamics images in the CuBiPSe/CN heterostructure.

MOF-Derived CoSe Nanoparticles/Carbonized Melamine Foam as Catalytic Cathode Enabling Flexible Li-CO Batteries with High Energy Efficiency and Stable Cycling.

Rechargeable aprotic Li-CO batteries have aroused worldwide interest owing to their environmentally friendly CO fixation ability and ultra-high specific energy density. However, its practical applications are impeded by the sluggish reaction kinetics and discharge product accumulation during cycling. Herein, a flexible composite electrode comprising CoSe nanoparticles embedded in 3D carbonized melamine foam (CoSe/CMF) for Li-CO batteries is reported.

Electrical Discharge in a Cavitating Liquid under an Ultrasound Field.

A theoretical model for an electrical discharge in a cavitating liquid is developed and compared with experiments for the optimization of the water treatment device. The calculations based on solution of the Noltingk─Neppiras equation support the hypothesis that the electric field promotes the formation of vapor microchannels inside a liquid gap between the electrodes, where at a low gas pressure Paschen's conditions of rupture and abnormal glow discharge maintenance in those microchannels are fulfilled. Theoretical analysis of the cavitation processes and the discharge formation processes is in qualitative agreement with the experimental data obtained in this work in a water treatment device using a hydrodynamic emitter.

Mn-Modified ZnO Nanoflakes for Optimal Photoelectrochemical Performance Under Visible Light: Experimental Design and Theoretical Rationalization.

Doping of zinc oxide (ZnO) with manganese (Mn) tunes midbandgap states of ZnO to enhance its optical properties and makes it into an efficient photoactive material for photoelectrochemical water splitting, waste removal from water, and other applications. We demonstrate that ZnO modified with 1 at. % Mn exhibits the best performance, as rationalized by experimental, structural, and optical characterization and theoretical analysis.