Fe-Single-Atom Incorporated Wood-Derived Anode with Fe─N─C/FeC Structural Unit and Hollow Diffusion Sites for Enhanced Sodium-Ion Storage.

Sluggish diffusion kinetics of Na drastically restrain the rate capability and capacitance of the anode for sodium-ion batteries (SIBs). Herein, a Fe single-atom strategy is employed to construct Fe─N─O active sites closely coupled with FeC species, establishing strong electronic interactions and, more importantly, an optimized coordination environment through precise tuning of their composition ratio with wood-derived nanoporous carbon (WNC) support. The charging Na through nanoporous carbon of Fe─N─O-WNC anode is revealed by electrochemical capacitive and charge-discharge studies to establish a reversible conversion and diffusion of Na supported by theoretical calculation of Na migration energy (eV) against the diffusion path.

Transition-Metal-Free Electrodes for Rechargeable Sodium-Ion Batteries: a Path towards Sustainable Energy Storage.

Development of sodium-ion batteries (SIBs) is of significant recent interest in energy storage in view of some positive aspects, such as the abundance of sodium over lithium, their fast-charging capability, cobalt-free cathode, safe transportability, etc. although with somewhat lower capacities. With numerous battery applications developing due to the new energy initiatives, SIBs are finding a niche place in this ecosystem.

Tunable Charge Distribution in Self-Supported NiCoP Through V and Mo Incorporation for Efficient Hydrogen Evolution in all pH Ranges and Alkaline Seawater.

Developing electrocatalysts with high activity and durability remains a key challenge in water electrolysis, essential for advancing sustainable hydrogen fuel production. Efficient electrocatalysts capable of functioning across diverse pH conditions and in alkaline seawater for hydrogen evolution reactions (HER) are crucial for the future of clean energy. In this study, a dual incorporation of vanadium (V) and molybdenum (Mo) into NiCoP [V, M (x,y)-NCP] catalyst is successfully fabricated via electrodeposition, offering an effective method for enhancing HER activity.

Architectural Innovations in Perovskite Solar Cells.

Meeting future energy demands with sustainable sources like photovoltaics (PV) presents significant land and logistical challenges, which can be mitigated by improving PV power conversion efficiency (PCE) and decentralized solutions like building-integrated photovoltaics and solar-integrated mobility systems (e.g., Unmanned Aerial Vehicles (UAVs)).

Quantitative Physiologic MRI Combined with Feature Engineering for Developing Machine Learning-Based Prediction Models to Distinguish Glioblastomas from Single Brain Metastases.

: The accurate and early distinction of glioblastomas (GBMs) from single brain metastases (BMs) provides a window of opportunity for reframing treatment strategies enabling optimal and timely therapeutic interventions. We sought to leverage physiologically sensitive parameters derived from diffusion tensor imaging (DTI) and dynamic susceptibility contrast (DSC)-perfusion-weighted imaging (PWI) along with machine learning-based methods to distinguish GBMs from single BMs. : Patients with histopathology-confirmed GBMs ( = 62) and BMs ( = 26) and exhibiting contrast-enhancing regions (CERs) underwent 3T anatomical imaging, DTI and DSC-PWI prior to treatment.

How the Kinetic Balance Between Charge-Transfer and Mass-Transfer Influences Zinc Anode Stability: An Ultramicroelectrode Study.

Aqueous zinc-metal batteries (AZMBs) represent a promising frontier in battery technology, offering sustainable and safe alternatives to traditional non-aqueous batteries. Despite their potential, understanding the kinetics of zinc electrodeposition-a critical factor in AZMB performance-remains underexplored. Utilizing voltammetry on ultramicroelectrodes, we investigate how scan rate influences key processes of nucleation and growth during Zn electrodeposition.

Lithium niobate on insulator: an emerging nanophotonic crystal for optimized light control.

Lithium niobate (LN) stands out as a versatile nonlinear optoelectronic material which can be directly applied in tunable modulators, filters, parametric amplifiers, and photonic integrated circuits. Recently, LN photonic crystals have garnered attention as a compelling candidate for incorporation into photonic integrated circuits, showcasing their potential in advancing the field. Photonic crystals possess a widely acknowledged capability to manipulate the transmission of light modes, similar to how nanostructures have been utilized to regulate electron-related phenomena.

Modulation of Electron Push-Pull by Redox Non-Innocent Additives for Long Cycle Life Zinc Anode.

Application of an aqueous Zn-ion battery is plagued by a water-induced hydrogen evolution reaction (HER), resulting in local pH variations and an unstable electrode-electrolyte interface (EEI) with uncontrolled Zn plating and side reactions. Here, 4-methyl pyridine N-oxide (PNO) is introduced as a redox non-innocent additive that comprises a hydrophilic bipolar N-O ion pair as a coordinating ligand for Zn and a hydrophobic ─CH group at the para position of the pyridine ring that reduces water activity at the EEI, thereby enhancing stability. The N-O moiety of PNO possesses the unique functionality of an efficient push electron donor and pull electron acceptor, thus maintaining the desired pH during charging/discharging.

Exploring the Complex Chemistry and Degradation of Ascorbic Acid in Aqueous Nanoparticle Synthesis.

Ascorbic acid (AA) is the most widely used reductant for noble metal nanoparticle (NP) synthesis. Despite the synthetic relevance, its aqueous chemistry remains misunderstood, due in part to various assumptions about its reduction pathway which are insufficiently supported by experimental evidence. This study aims to provide an understanding of the complex chemistry associated with AA under aqueous conditions.

Reverse Intersystem Crossing Dynamics in Vibronically Modulated Inverted Singlet-Triplet Gap System: A Wigner Phase Space Study.

We inspect the origin of the inverted singlet-triplet gap (INVEST) and slow change in the reverse intersystem crossing (rISC) rate with temperature, as recently observed. A Wigner phase space study reveals that, though INVEST is found at equilibrium geometry, variation in the exchange interaction and the doubles-excitation for other geometries in the harmonic region leads to non-INVEST behavior. This highlights the importance of nuclear degrees of freedom for the INVEST phenomenon, and in this case, geometric puckering of the studied molecule determines INVEST and the associated rISC dynamics.

Dimerization of Fe(III) Ion in an Aqueous Medium: Mechanistic Modelling and Effects of Ligands.

Aqueous iron solutions generally undergo spontaneous hydrolysis followed by aggregation resulting in the precipitation of nanocrystalline oxyhydroxide minerals. The mechanism of nucleation of such multinuclear oxyhydroxide clusters are unclear due to limited experimental evidence. Here, we investigate the mechanistic pathway of dimerization of Fe(III) ions using density functional theory (DFT) in aqueous medium considering effects of other ligands.

Exploring Layered Disorder in Lithium-Ion-Conducting LiYInCl.

LiYInCl undergoes a phase transition from trigonal to monoclinic via an intermediate orthorhombic phase. Although the trigonal yttrium containing the end member phase, LiYCl, synthesized by a mechanochemical route, is known to exhibit stacking fault disorder, not much is known about the monoclinic phases of the serial composition LiYInCl. This work aims to shed light on the influence of the indium substitution on the phase evolution, along with the evolution of stacking fault disorder using X-ray and neutron powder diffraction together with solid-state nuclear magnetic resonance spectroscopy, studying the lithium-ion diffusion.

H-Glass Supported Hybrid Gold Nano-Islands for Visible-Light-Driven Hydrogen Evolution.

Flat panel reactors, coated with photocatalytic materials, offer a sustainable approach for the commercial production of hydrogen (H) with zero carbon footprint. Despite this, achieving high solar-to-hydrogen (STH) conversion efficiency with these reactors is still a significant challenge due to the low utilization efficiency of solar light and rapid charge recombination. Herein, hybrid gold nano-islands (HGNIs) are developed on transparent glass support to improve the STH efficiency.

Design and Piezoelectric Energy Harvesting Properties of a Ferroelectric Cyclophosphazene Salt.

Cyclophosphazenes offer a robust and easily modifiable platform for a diverse range of functional systems that have found applications in a wide variety of areas. Herein, for the first time, it reports an organophosphazene-based supramolecular ferroelectric [(PhCH NH) P N Me]I, [PMe]I. The compound crystallizes in the polar space group Pc and its thin-film sample exhibits remnant polarization of 5 µC cm .

Mitigating Dendrite Formation on a Zn Electrode in Aqueous Zinc Chloride by the Competitive Surface Chemistry of an Imidazole Additive.

Electrochemical energy storage systems are critical in several ways for a smooth transition from nonrenewable to renewable energy sources. Zn-based batteries are one of the promising alternatives to the existing state-of-the-art Li-ion battery technology, since Li-ion batteries pose significant drawbacks in terms of safety and cost-effectiveness. Zn (with a reduction potential of -0.

Adiabatic state preparation of correlated wave functions with nonlinear scheduling functions and broken-symmetry wave functions.

Adiabatic state preparation (ASP) can generate the correlated wave function by simulating the time evolution of wave function under the time-dependent Hamiltonian that interpolates the Fock operator and the full electronic Hamiltonian. However, ASP is inherently unsuitable for studying strongly correlated systems, and furthermore practical computational conditions for ASP are unknown. In quest for the suitable computational conditions for practical applications of ASP, we performed numerical simulations of ASP in the potential energy curves of N, BeH, and in the C quasi-reaction pathway of the Be atom insertion to the H molecule, examining the effect of nonlinear scheduling functions and the ASP with broken-symmetry wave functions with the S operator as the penalty term, contributing to practical applications of quantum computing to quantum chemistry.

Quantum Algorithm for Numerical Energy Gradient Calculations at the Full Configuration Interaction Level of Theory.

A Bayesian phase difference estimation (BPDE) algorithm allows us to compute the energy gap of two electronic states of a given Hamiltonian directly by utilizing the quantum superposition of their wave functions. Here we report an extension of the BPDE algorithm to the direct calculation of the energy difference of two molecular geometries. We apply the BPDE algorithm for the calculation of numerical energy gradients based on the two-point finite-difference method, enabling us to execute geometry optimization of one-dimensional molecules at the full-CI level on a quantum computer.

Efficient Nitrate Conversion to Ammonia on f-Block Single-Atom/Metal Oxide Heterostructure Local Electron-Deficiency Modulation.

Exploring single-atom catalysts (SACs) for the nitrate reduction reaction (NO; NitRR) to value-added ammonia (NH) offers a sustainable alternative to both the Haber-Bosch process and NO-rich wastewater treatment. However, due to the insufficient electron deficiency and unfavorable electronic structure of SACs, resulting in poor NO-adsorption, sluggish proton (H*) transfer kinetics, and preferred hydrogen evolution, their NO-to-NH selectivity and yield rate are far from satisfactory. Herein, a systematic theoretical prediction reveals that the local electron deficiency of an -block Gd single atom (Gd) can be significantly regulated upon coordination with oxygen-defect-rich NiO (Gd-D-NiO) support.

Construction of a 2D/2D g-CN/NiCr-LDH Heterostructure to Boost the Green Ammonia Production Rate under Visible Light Illumination.

Photocatalytic N fixation has emerged as one of the most useful ways to produce NH, a useful asset for chemical industries and a carbon-free energy source. Recently, significant progress has been made toward designing efficient photocatalysts to achieve this objective. Here, we introduce a highly active type-II heterojunction fabricated via integrating two-dimensional (2D) nanosheets of exfoliated g-CN with nickel-chromium layered double hydroxide (NiCr-LDH).

Search for New Anode Materials for High Performance Li-Ion Batteries.

Owing to an unmatched combination of power and energy density along with cyclic stability, the Li-ion battery has qualified itself to be the highest performing rechargeable battery. Taking both transportable and stationary energy storage requirements into consideration, Li-ion batteries indeed stand tall in comparison to any other existing rechargeable battery technologies. However, graphite, which is still one of the best performing Li-ion anodes, has specific drawbacks in fulfilling the ever-increasing energy and power density requirements of the modern world.

Efficient Piezoelectric Energy Harvesting from a Discrete Hybrid Bismuth Bromide Ferroelectric Templated by Phosphonium Cation.

Bismuth containing hybrid molecular ferroelectrics are receiving tremendous attention in recent years owing to their stable and non-toxic composition. However, these perovskite-like structures are primarily limited to ammonium cations. Herein, we report a new phosphonium based discrete perovskite-like hybrid ferroelectric with a formula [Me(Ph) P] [Bi Br ] (MTPBB) and its mechanical energy harvesting capability.

Variational quantum eigensolver simulations with the multireference unitary coupled cluster ansatz: a case study of the quasi-reaction pathway of beryllium insertion into a H molecule.

Variational quantum eigensolver (VQE)-based quantum chemical calculations have been extensively studied as a computational model using noisy intermediate-scale quantum devices. The VQE uses a parametrized quantum circuit defined through an "ansatz" to generate approximated wave functions, and the appropriate choice of an ansatz is the most important step. Because most chemistry problems focus on the energy difference between two electronic states or structures, calculating the total energies in different molecular structures with the same accuracy is essential to correctly understand chemistry and chemical processes.

Growth of highly conducting MoSN thin films with enhanced 1T' phase by pulsed laser deposition and exploration of their nanogenerator application.

High-quality growth of MoSN films is realized on single-crystal -AlO substrates by the pulsed laser deposition (PLD) in ammonia rendering highly stable and tunable 1T'/2H biphasic constitution. Raman spectroscopy reveals systematic enhancement of 1T' phase component due to the incorporation of covalently bonded N-doping in MoS lattice, inducing compressive strain. Interestingly, the film deposited at 300 mTorr NH shows ∼80% 1T' phase.

Visible Light-Driven Highly Selective CO Reduction to CH Using Potassium-Doped g-CN.

Establishment of an efficient and robust artificial photocatalytic system to convert solar energy into chemical fuels through CO conversion is a cherished goal in the fields of clean energy and environmental protection. In this work, we have explored an emergent low- nitrogen-rich carbon nitride material g-CN (analogue of g-CN) for CO conversion under visible light illumination. A significant enhancement of the CH production rate was detected for g-CN in comparison to that of g-CN.

Quantum Algorithm for Full Configuration Interaction Calculations without Controlled Time Evolutions.

A quantum phase estimation algorithm allows us to perform full configuration interaction (full-CI) calculations on quantum computers with polynomial costs against the system size under study, but it requires quantum simulation of the time evolution of the wave function conditional on an ancillary qubit, which makes the algorithm implementation on real quantum devices difficult. Here, we discuss an application of the Bayesian phase difference estimation algorithm that is free from controlled time evolution operations to the full-CI calculations.