Boosting the interfacial dynamics and thermodynamics in polyanion cathode by carbon dots for ultrafast-charging sodium ion batteries.

Ultrafast-charging is the focus of next-generation rechargeable batteries for widespread economic success by reducing the time cost. However, the poor ion diffusion rate, intrinsic electronic conductivity and structural stability of cathode materials seriously hinder the development of ultrafast-charging technology. To overcome these challenges, an interfacial dynamics and thermodynamics synergistic strategy is proposed to synchronously enhance the fast-charging capability and structural stability of polyanion cathode materials.

Trapping Lithium Selenides with Evolving Heterogeneous Interfaces for High-Power Lithium-Ion Capacitors.

Transition metal selenides anodes with fast reaction kinetics and high theoretical specific capacity are expected to solve mismatched kinetics between cathode and anode in Li-ion capacitors. However, transition metal selenides face great challenges in the dissolution and shuttle problem of lithium selenides, which is the same as Li-Se batteries. Herein, inspired by the density functional theory calculations, heterogeneous can enhance the adsorption of Li Se relative to single component selenide electrodes, thus inhibiting the dissolution and shuttle effect of Li Se.

Cationic-potential tuned biphasic layered cathodes for stable desodiation/sodiation.

Sodium layered oxides generally suffer from deep-desodiation instability in P2 structure and sluggish kinetics in O3 structure. It will be great to design P2/O3 biphasic materials that bring the complementary merits of both structures. However, such exploration is hindered by the ambiguous mechanism of material formation.

Metal-Organic Framework Materials for Electrochemical Supercapacitors.

Exploring new materials with high stability and capacity is full of challenges in sustainable energy conversion and storage systems. Metal-organic frameworks (MOFs), as a new type of porous material, show the advantages of large specific surface area, high porosity, low density, and adjustable pore size, exhibiting a broad application prospect in the field of electrocatalytic reactions, batteries, particularly in the field of supercapacitors. This comprehensive review outlines the recent progress in synthetic methods and electrochemical performances of MOF materials, as well as their applications in supercapacitors.

Ultra-Low-Dose Pre-Metallation Strategy Served for Commercial Metal-Ion Capacitors.

Interfacial bonding strategy has been successfully applied to address the high overpotential issue of sacrificial additives, which reduced the decompositon potential of NaCO from 4.50 to 3.95 V.

New insights of QTAIM and stress tensor to finding non-competitive/competitive torquoselectivity of cyclobutene.

This study aims to investigate the phenomenon of torquoselectivity through three thermal cyclobutene ring-opening reactions (N1-N3). This research focuses on the nature of the chemical bond, electronic reorganization, predicting non-competitive or competitive reactions, and torquoselectivity preference within Quantum Theory of Atoms in Molecules (QTAIM) and stress tensor frameworks. Various theoretical analyses for these reactions, such as metallicity ξ(r), ellipticity ε, total local energy density H(r), stress tensor polarizability ℙ, stress tensor eigenvalue λ, and bond-path length, display differently for non-competitive and competitive reactions as well as for the conrotatory preferences either it is the transition state outward conrotatory (TS) or transition state inward conrotatory (TS) directions by presenting degeneracy or non-degeneracy in their results.

High content anion (S/Se/P) doping assisted by defect engineering with fast charge transfer kinetics for high-performance sodium ion capacitors.

The rate-determining process for sodium storage in TiO is greatly depending on charge transfer happening in the electrode materials owing to its inferior diffusion coefficient and electronic conductivity. Apart from reducing the diffusion distance of ion/electron, the increasement of ionic/electronic mobility in the crystal lattice is also very important for charge transport. Here, an oxygen vacancy (OV) engineering assisted in high-content anion (S/Se/P) doping strategy to enhance charge transfer kinetics for ultrafast sodium-storage performance is proposed.

Next-generation QTAIM for scoring molecular wires in E-fields for molecular electronic devices.

The effect of a varying, directional E , E , and E electric field on the ethene molecule was investigated using next-generation quantum theory of atoms in molecules (QTAIM). Despite using low E-field strengths that are within the realm of experiment and do not measurably alter the molecular geometry, significant changes to the QTAIM properties were observed. Using conventional QTAIM, the shifting of the C─C and C─H bond critical points (BCPs) demonstrates polarization through an interchange in the size of the atoms involved in a bond, since a BCP is located on the boundary between a pair of bonded atoms.

3-D bond-paths of QTAIM and the stress tensor in neutral lithium clusters, Li (m = 2-5), presented on the Ehrenfest force molecular graph.

In this investigation we set out to understand the origins of non-nuclear attractors (NNAs) found for neutral lithium clusters Lim (m = 2-5) on the QTAIM molecular graph but not on the Ehrenfest force F(r) molecular graph. Therefore, we pursued the stress tensor σ(r) without using the dependency on the QTAIM partitioning, since previously σ(r) was only calculated within the QTAIM partitioning, to see if any indication of NNA character can be determined. Because the stress tensor σ(r) lacks an associated scalar- or vector-field as is the case for QTAIM and the Ehrenfest F(r) partitioning schemes respectively, a stress tensor σ(r) partitioning scheme cannot be constructed.

Stress Tensor Eigenvector Following with Next-Generation Quantum Theory of Atoms in Molecules: Excited State Photochemical Reaction Path from Benzene to Benzvalene.

In this investigation, we considered both the scalar and 3-D vector-based measures of bonding using next generation quantum theory of atoms in molecules (QTAIM), constructed from the preferred direction of electronic charge density accumulation, to better understand the photochemical reaction associated with of the formation of benzvalene from benzene. The formation of benzvalene from benzene resulted in two additional C-C bonds forming compared with the benzene. The creation of the additional C-C bonds was explained in terms of an increasing the favorability of the reaction process by maximizing the bonding density.

The destabilization of hydrogen bonds in an external E-field for improved switch performance.

The effect of an electric field on a recently proposed molecular switch based on a quinone analogue was investigated using next-generation quantum theory of atoms in molecules (QTAIM) methodology. The reversal of a homogenous external electric field was demonstrated to improve the "OFF" functioning of the switch. This was achieved by destabilization of the H atom participating in the tautomerization process along the hydrogen bond that defines the switch.

Chirality-Helicity Equivalence in the S and R Stereoisomers: A Theoretical Insight.

We located the unknown chirality-helicity equivalence in molecules with a chiral center, and as a consequence, the degeneracy of the S and R stereoisomers of lactic acid was lifted. An agreement was found with the naming schemes of S and R stereoisomers from optical experiments. This was made possible by the construction of the stress tensor trajectories in a non-Cartesian space defined by the variation of the position of the torsional bond critical point upon a structural change, along the torsion angle, θ, involving a chiral carbon atom.

Non-nuclear attractors in small charged lithium clusters, Li (m = 2-5, q = ±1), with QTAIM and the Ehrenfest force partitioning.

In this investigation we explore the function and existence of the non-nuclear attractor (NNA) for a series of small charged lithium clusters Limq (m = 2-5, q = ±1) using QTAIM and the Ehrenfest force F(r) partitioning schemes. The NNAs were found to be present in all of the Limq (m = 2-5, q = ±1) clusters for QTAIM, in contrast none were found for F(r). We discovered that the anionic and cationic lithium dimers are limiting cases for minimal and maximal impact of the NNA related to the relative sparseness of total charge density ρ(r) distributions respectively.

Exploration of the forbidden regions of the Ramachandran plot (ϕ-ψ) with QTAIM.

A new QTAIM interpretation of the Ramachandran plot is formulated from the most and least facile eigenvectors of the second-derivative matrix of the electron density with a set of 29 magainin-2 peptide conformers. The presence of QTAIM eigenvectors associated with the most and least preferred directions of electronic charge density explained the role of hydrogen bonding, HH contacts and the glycine amino acid monomer in peptide folding. The highest degree of occupation of the QTAIM interpreted Ramachandran plot was found for the glycine amino acid monomer compared with the remaining backbone peptide bonds.

QTAIM and Stress Tensor Characterization of Intramolecular Interactions Along Dynamics Trajectories of a Light-Driven Rotary Molecular Motor.

A quantum theory of atoms in molecules (QTAIM) and stress tensor analysis was applied to analyze intramolecular interactions influencing the photoisomerization dynamics of a light-driven rotary molecular motor. For selected nonadiabatic molecular dynamics trajectories characterized by markedly different S state lifetimes, the electron densities were obtained using the ensemble density functional theory method. The analysis revealed that torsional motion of the molecular motor blades from the Franck-Condon point to the S energy minimum and the S/S conical intersection is controlled by two factors: greater numbers of intramolecular bonds before the hop-time and unusually strongly coupled bonds between the atoms of the rotor and the stator blades.

Distinguishing and quantifying the torquoselectivity in competitive ring-opening reactions using the stress tensor and QTAIM.

Currently the theories to explain and predict the classification of the electronic reorganization due to the torquoselectivity of a ring-opening reaction cannot accommodate the directional character of the reaction pathway; the torquoselectivity is a type of stereoselectivity and therefore is dependent on the pathway. Therefore, in this investigation we introduced new measures from quantum theory of atoms in molecules and the stress tensor to clearly distinguish and quantify the transition states of the inward (TSIC) and outward (TSOC) conrotations of competitive ring-opening reactions of 3-(trifluoromethyl)cyclobut-1-ene and 1-cyano-1-methylcyclobutene. We find the metallicity ξ(r ) of the ring-opening bond does not occur exactly at the transition state in agreement with transition state theory.

QTAIM and stress tensor interpretation of the (H O) potential energy surface.

Using the quantum theory of atoms in molecules a near complete combined directed spanning quantum topology phase diagram (QTPD) was constructed from the nine (H O) reaction-pathways and five unique Poincaré-Hopf solutions that were found after an extensive search of the MP2 potential energy surface. Two new energy minima that were predicted from earlier work are found and include the first (H O) conformer with a 3-D quantum topology. The stress tensor Poincaré-Hopf relation indicated a preference for 2-D (H O) topologies as well as the presence of coupling between shared-shell OH BCPs to the hydrogen-bond BCPs that share an H NCP.

A QTAIM and stress tensor investigation of the torsion path of a light-driven fluorene molecular rotary motor.

The utility of the QTAIM/stress tensor analysis method for characterizing the photoisomerization of light driven molecular rotary machines is investigated on the example of the torsion path in fluorene molecular motor. The scalar and vector descriptors of QTAIM/stress tensor reveal additional information on the bonding interactions between the rotating units of the motor, which cannot be obtained from the analysis of the ground and excited state potential energy surfaces. The topological features of the fluorene motor molecular graph display that, upon the photoexcitation a certain increase in the torsional stiffness of the rotating bond can be attributed to the increasing topological stability of the rotor carbon atom attached to the rotation axle.