Interfacial degradation of PEO-based polymer electrolytes on the NMC cathode and CEI components prediction.

All-solid-state Li-metal batteries using solid polymer electrolytes (SPEs) in combination with high-voltage cathodes such as lithium nickel manganese cobalt oxide (NMC) promise enhanced battery safety, energy density, and flexibility. However, understanding the oxidative decomposition of SPEs on the cathode surfaces and characterizing the resulting cathode-electrolyte interphase (CEI) remain challenging both experimentally and computationally. This study introduces a new computational protocol based on ab initio molecular dynamics for simulating the decomposition of PEO:LiTFSI SPE on the NMC-811 cathode surface using a combined electron- and Li+-removal simulation approach.

Multifunctional Zwitterionic Self-Healing Polymer Electrolytes for Anode-Free Lithium-Metal Batteries: a Computational Perspective.

The practical application of anode-free lithium-metal batteries (AFLMBs) is limited by their poor cycling performance and unstable solid electrolyte interphase (SEI). Self-healing solid polymer electrolytes (SHSPEs) offer excellent flexibility and healing capabilities, which are expected to mitigate dendrite growth and improve AFLMB cycling performance. In this study, a novel zwitterionic SHSPE, P(SBMA-co-BA):LiTFSI, is proposed, and its suitability for AFLMBs is evaluated through density functional theory (DFT) and ab initio molecular dynamics (AIMD) simulations.

Enhancing Anode-Free Battery Performance with Self-Healing Single-Ion Conducting PAMPS--PBA Copolymer Interfaces.

The design of anode-free batteries presents an attractive approach to the lithium metal battery. However, challenges such as uneven plating of lithium and poor Coulombic efficiency limit their commercially viable applications. In response to these challenges, this study introduces poly{(2-acrylamido-2-methylpropanesulfonic acid)--(butyl acrylate)} (PAMPS--PBA), an artificial interface engineered to enhance the cyclic stability of batteries by fortifying the solid electrolyte interphase (SEI) and enabling self-healing and single-ion conductivity.

Enhancing optical absorbance and accelerating rotational speed in molecular motors through oriented external electric fields.

Accelerating the rotational speed of light-driven molecular motors is among the foremost concerns in molecular machine research, as this speed directly influences the performance of a motor. Controlling the motor's rotation is crucial for practical applications, and using an oriented external electric field (OEEF) represents a feasible method to achieve this objective. We have investigated the impact of an OEEF on the optical and kinetic properties of a novel π-donor/acceptor di-substituted molecular motor, R2,3-(NH2, CHO).

Unraveling the catalytic performance of RuO(1 1 0) for highly-selective ethylene production from methane at low temperature: Insights from first-principles and microkinetic simulations.

Despite significant progress in low-temperature methane (CH) activation, commercial viability, specifically obtaining high yields of C/C products, remains a challenge. High desorption energy (>2 eV) and overoxidation of the target products are key limitations in CH utilization. Herein, we employ first-principles density functional theory (DFT) and microkinetics simulations to investigate the CH activation and the feasibility of its conversion to ethylene (CH) on the RuO (1 1 0) surface.

Initial SEI formation in LiBOB-, LiDFOB- and LiBF-containing PEO electrolytes.

A limiting factor for solid polymer electrolyte (SPE)-based Li-batteries is the functionality of the electrolyte decomposition layer that is spontaneously formed at the Li metal anode. A deeper understanding of this layer will facilitate its improvement. This study investigates three SPEs - polyethylene oxide:lithium tetrafluoroborate (PEO:LiBF), polyethylene oxide:lithium bis(oxalate)borate (PEO:LiBOB), and polyethylene oxide:lithium difluoro(oxalato)borate (PEO:LiDFOB) - using a combination of electrochemical impedance spectroscopy (EIS), galvanostatic cycling, Li deposition photoelectron spectroscopy (PES), and molecular dynamics (AIMD) simulations.

The use of multicomponent reactions in the development of bis-boronic acids for the detection of β-sialic acid.

Sialic acid (SA) is a naturally occurring monosaccharide found in glycoproteins and glycolipids. Changes in the expression of SA are associated with several diseases; thus, the detection of SA is of great significance for biological research, cancer diagnosis, and treatment. Boronic acid analogs have emerged as a promising tool for detecting sugars such as SA due to its reversible covalent bonding ability.

Lewis Acid Probe for Basicity of Sulfide Electrolytes Investigated by B Solid-State NMR.

Sulfide-based solid-state lithium-ion batteries (SSLIB) have attracted a lot of interest globally in the past few years for their high safety and high energy density over the traditional lithium-ion batteries. However, sulfide electrolytes (SEs) are moisture-sensitive which pose significant challenges in the material preparation and cell manufacturing. To the best of our knowledge, there is no tool available to probe the types and the strength of the basic sites in sulfide electrolytes, which is crucial for understanding the moisture stability of sulfide electrolytes.

Synergistic dual electrolyte additives for fluoride rich solid-electrolyte interface on Li metal anode surface: Mechanistic understanding of electrolyte decomposition.

Improving the quality of the solid-electrolyte interphase (SEI) layer is highly imperative to stabilize the Li-metal anodes for the practical application of high-energy-density batteries. However, controllably managing the formation of robust SEI layers on the anode is challenging in state-of-the-art electrolytes. Herein, we discuss the role of dual additives fluoroethylene carbonate (FEC) and lithium difluorophosphate (LiPOF, LiPF) within the commercial electrolyte mixture (LiPF/EC/DEC) considering their reactivity with Li metal anodes using density functional theory (DFT) and ab initio molecular dynamics (AIMD) simulations.

Exploiting High-Voltage Stability of Dual-Ion Aqueous Electrolyte Reinforced by Incorporation of Fiberglass into Zwitterionic Hydrogel Electrolyte.

Rechargeable zinc aqueous batteries are key alternatives for replacing toxic, flammable, and expensive lithium-ion batteries in grid energy storage systems. However, these systems possess critical weaknesses, including the short electrochemical stability window of water and intrinsic fast zinc dendrite growth. Hydrogel electrolytes provide a possible solution, especially cross-linked zwitterionic polymers that possess strong water retention ability and high ionic conductivity.

A method for modelling polymer electrolyte decomposition during the Li-nucleation process in Li-metal batteries.

Elucidating the complex degradation pathways and formed decomposition products of the electrolytes in Li-metal batteries remains challenging. So far, computational studies have been dominated by studying the reactions at inert Li-metal surfaces. In contrast, this study combines DFT and AIMD calculations to explore the Li-nucleation process for studying interfacial reactions during Li-plating by introducing Li-atoms close to the metal surface.

The remarkable performance of a single iridium atom supported on hematite for methane activation: a density functional theory study.

Methane is the major component of natural gas, and it significantly contributes to global warming. In this study, we investigated methane activation on the α-FeO(110) surface and M/α-FeO(110) surfaces (M = Ag, Ir, Cu, or Co) using the density-functional theory (DFT) + method. Our study shows that the Ir/α-FeO(110) surface is a more effective catalyst for C-H bond activation than other catalyst surfaces.

Theoretical insight into hydroxyl production HO decomposition over the FeO(311) surface.

Fenton's reagent provides a method to produce active hydroxyl radicals (˙OH) for chemical oxidation by mixing iron oxide and hydrogen peroxide, which divides into homogeneous and heterogeneous Fenton's reagent. Heterogeneous Fenton's reagent is fabricated from HO and various iron oxide solid materials, such as α-FeOOH, α-FeO, and FeO. FeO possesses the Fe/Fe mixed valence oxidational state and has been reported to have good catalytic activity.

The investigation of methane storage at the Ni-MOF-74 material: a periodic DFT calculation.

To develop a high-performance methane storage material, an understanding of the mechanism and electronic interactions between methane and the material is essential. In this study, we performed detailed theoretical analyses to investigate the methane storage capacity of Ni-MOF-74 using a large-scale periodic DFT code CONQUEST. In a single pore of the unit cell, we considered three possible sites, iSBU, L, and P sites, where iSBU is the inorganic secondary building unit with a metal center, and L is the linker consisting of the organic building unit, while the P site is the vacuum site in the center of the pore.

Combined Density Functional Theory and Microkinetics Study to Predict Optimum Operating Conditions of Si(100) Surface Carbonization by Acetylene for High Power Devices.

The Si(100) surface carbonization mechanisms by acetylene are explored using density functional theory calculations combined with microkinetic simulations. The most stable acetylene adsorption geometries and their subsequent decomposition mechanisms to form a carbon dimer on the Si surface are investigated. Microkinetics simulations are further used to examine the optimal reaction conditions for obtaining a single-crystalline silicon carbide (SiC).

New Insights into the N-S Bond Formation of a Sulfurized-Polyacrylonitrile Cathode Material for Lithium-Sulfur Batteries.

Sulfurized polyacrylonitrile (S-cPAN) has been recognized as a particularly promising cathode material for lithium-sulfur (Li-S) batteries due to its ultra-stable cycling performance and high degree of sulfur utilization. Though the synthetic conditions and routes for modification of S-cPAN have been extensively studied, details of the molecular structure of S-cPAN remain yet unclear. Herein, a more reasonable molecular structure consisting of pyridinic/pyrrolic nitrogen (N/N) is proposed, based on the analysis of combined X-ray photoelectron spectroscopy, C/N solid-state nuclear magnetic resonance, and density functional theory data.

Theoretical study on the interaction of iodide electrolyte/organic dye with the TiO surface in dye-sensitized solar cells.

The iodide/triiodide interaction with the dye on a semiconductor surface plays a significant role in understanding the dye-sensitized solar cells (DSSCs) mechanism and improving its efficiency. In the present study, density functional theory (DFT) calculations were used to determine the interaction between the complexed iodide redox couple with dye/TiO2 for the relevance of DSSCs. Three new metal-free organic dyes noted as D1Y, D2Y and D3Y, featured with D-π-A configuration were designed by varying functional groups on the donor moiety.

Enhanced moisture stability of cesium lead iodide perovskite solar cells - a first-principles molecular dynamics study.

An understanding of the interaction of water with perovskite is crucial in improving the structural stability of the perovskite. Hence, in this study, the structural and electronic properties of the γ-CsPbI(220) perovskite surface upon the adsorption of water molecules have been investigated based on density functional theory calculations. Also, we perform first-principles ab initio molecular dynamics simulations (AIMD) to explore the structural stability of the γ-CsPbI(220) perovskite surface in the presence of water molecules, and the results are compared with the conventional cubic CHNHPbI(100) perovskite surface.

B, N-co-doped graphene-supported Ir and Pt clusters for methane activation and C─C coupling: A density functional theory study.

Methane conversion by using transition metal catalysts plays in an important role in various usages of the industrial process. The mechanism of methane conversion on B, N-co-doped graphene supported Ir and Pt clusters, BNG-Ir4 and BNG-Pt4, have been investigated using density functional theory calculations. Methane was found to adsorb on BNG-Ir4 and BNG-Pt4 clusters via strong agostic interactions.

Understanding the Role of Dopant Metal Atoms on the Structural and Electronic Properties of Lithium-Rich LiNiMnO Cathode Material for Lithium-Ion Batteries.

Improving the stability of lithium-rich cathode materials is important in refining the overall performance of lithium-ion batteries. Here, we have proposed doping of different metal atoms such as K, Ca, Cd, and Al in different sites of LiNiMnO, and we have investigated their structural and electronic properties using first-principles calculations. We found that the Ni ions in the pristine LiNiMnO structure maintained the +3 oxidation state for a longer time and resulted in the structural deformation during the long cycling process.

Theoretical Study of Electrochemical and Electrochromic Properties of Novel Viologen Derivatives: Effects of Donors and π-Conjugation.

We propose a linkage approach by merging ambipolar electrochromic (EC) materials in both π-acceptor-π (π-A-π) and donor-acceptor-donor (D-A-D) configurations and investigated their electrochemical and spectroelectrochemical properties using density functional theory calculations. Here, we considered anthracene, toluene, and pyrene as π-conjugated molecules, triphenylamine (TPA) as a donor, and viologen as an acceptor moiety for π-A-π and D-A-D configurations. We have also explored the substitutional effects in the donor moiety on the overall electrochromism during both oxidation and reduction processes.

Temperature-programmed desorption studies of NH and HO on the RuO(110) surface: effects of adsorbate diffusion.

Temperature-programmed desorption (TPD) is one of the most straightforward surface science experiments for the determination of the thermodynamic and kinetic parameters of a reaction. In our previous study (J. Phys.

Effects of the terminal donor unit in dyes with D-D-π-A architecture on the regeneration mechanism in DSSCs: a computational study.

This theoretical study on dye-sensitized solar cells (DSSCs) includes design strategies for dye donor units to improve the efficiency of DSSCs, and further illuminates the organic dye regeneration mechanism. We have designed a series of new organic sensitizers based on a D-D-π-A architecture to exhibit easy electron transfer and to have remarkable light harvesting properties in the visible region by density functional theory (DFT) and time-dependent (TD)-DFT calculations. Furthermore, the interaction of the organic sensitizers with the conventional redox electrolyte using the triiodide/iodide couple (I3-/I-) is investigated.

Methanol decomposition reactions over a boron-doped graphene supported Ru-Pt catalyst.

The decomposition of methanol is currently attracting research attention due to the potential widespread applications of its end products. In this work, density functional theory (DFT) calculations have been performed to investigate the adsorption and decomposition of methanol on a Ru-Pt/boron doped graphene surface. We find that the most favorable reaction pathway is methanol (CH3OH) decomposition through O-H bond breaking to form methoxide (CH3O) as the initial step, followed by further dehydrogenation steps which generate formaldehyde (CH2O), formyl (CHO), and carbon monoxide (CO).