Gas solubility in ionic liquids.

Lithium-sulfur (Li-S) batteries have been intensively concerned to fulfill the urgent demands of high capacity energy storage. One of the major unsolved issues is the complex diffusion of lithium polysulfide intermediates, which in combination with the subsequent paradox reactions is known as the shuttle effect. Nanocarbon with homogeneous nonpolar surface served as scaffolding materials in sulfur cathode basically cannot afford a sufficient binding and confining effect to maintain lithium polysulfides within the cathode. Herein, a systematical density functional theory calculation of various heteroatoms-doped nanocarbon materials is conducted to elaborate the mechanism and guide the future screening and rational design of Li-S cathode for better performance. It is proved that the chemical modification using N or O dopant significantly enhances the interaction between the carbon hosts and the polysulfide guests via dipole-dipole electrostatic interaction and thereby effectively prevents shuttle of polysulfides, allowing high capacity and high coulombic efficiency. By contrast, the introduction of B, F, S, P, and Cl monodopants into carbon matrix is unsatisfactory. To achieve the strong-couple effect toward Li2 Sx , the principles for rational design of doped carbon scaffolds in Li-S batteries to achieve a strong electrostatic dipole-dipole interaction are proposed. An implicit volcano plot is obtained to describe the dependence of binding energies on electronegativity of dopants. Moreover, the codoping strategy is predicted to achieve even stronger interfacial interaction to trap lithium polysulfides.

Design Principles for Heteroatom-Doped Nanocarbon to Achieve Strong Anchoring of Polysulfides for Lithium-Sulfur Batteries.

The conductor-like screening model for realistic solvation (COSMO-RS) method has been established as a novel way to predict thermophysical data for liquid systems and has become a frequently used alternative to force field-based molecular simulation methods on one side and group contribution methods on the other. Through its unique combination of a quantum chemical treatment of solutes and solvents with an efficient statistical thermodynamics procedure for the molecular surface interactions, it enables the efficient calculation of many properties that other methods can barely predict. This review presents a short delineation of the theory, the application potential and limitations of COSMO-RS, and its most important application areas.

COSMO-RS: An Alternative to Simulation for Calculating Thermodynamic Properties of Liquid Mixtures

The continuously increasing CO2 released from human activities poses a great threat to human survival by fluctuating global climate and disturbing carbon balance among the four reservoirs of the biosphere, earth, air, and water. Converting CO2 to value-added feedstocks via electrocatalysis of the CO2 reduction reaction (CO2RR) has been regarded as one of the most attractive routes to re-balance the carbon cycle, thanks to its multiple advantages of mild operating conditions, easy handling, tunable products and the potential of synergy with the rapidly increasing renewable energy (i.e., solar, wind). Instead of focusing on a special topic of electrocatalysts for the CO2RR that have been extensively reviewed elsewhere, we herein present a rather comprehensive review of the recent research progress, in the view of associated value-added products upon selective electrocatalytic CO2 conversion. We initially provide an overview of the history and the fundamental science regarding the electrocatalytic CO2RR, with a special introduction to the design, preparation, and performance evaluation of electrocatalysts, the factors influencing the CO2RR, and the associated theoretical calculations. Emphasis will then be given to the emerging trends of selective electrocatalytic conversion of CO2 into a variety of value-added products. The structure-performance relationship and mechanism will also be discussed and investigated. The outlooks for CO2 electrocatalysis, including the challenges and opportunities in the development of new electrocatalysts, electrolyzers, the recently rising operando fundamental studies, and the feasibility of industrial applications are finally summarized.

Electrocatalysis for CO2 conversion: from fundamentals to value-added products

Theoretical insight into an empirical rule about organic corrosion inhibitors containing nitrogen, oxygen, and sulfur atoms

The DMol3 COSMO method is revisited and generalized for infinite polymer and surface models with periodic boundary conditions The procedure works also for three dimensionally periodic solid models with internal surfaces A new solvent accessible surface grid construction is presented, where the grid points and weights are a continuous function for all atomic geometries The calculated solvation energy is also continuous by consequence, which is useful for all calculations which involve geometry changes of the atomic framework The new method is tested with a few examples

The conductor-like screening model for polymers and surfaces

Unrelaxed surface models of several relevant faces of the two polymorphic forms of paracetamol were studied by DMol3‐conductor-like screening model (COSMO) calculations. This is a computationally expedient first step towards a more complete study of wettability. Our calculated wetting energies for the different faces show a trend consistent with recent contact angle measurements for paracetamol and water. The orthorhombic (0 0 1) and the monoclinic (0 1 0) surfaces are the most stable ones in the dry state as well as in the wet state. The COSMO wetting energy for these two surfaces agrees very well with the values deduced from experiment. The calculated COSMO wetting energies for the other, more polar, surfaces are higher and get overestimated by the model.

B. Delley

Papers

The conductor-like screening model for polymers and surfaces

Wetting of paracetamol surfaces studied by DMol3‐COSMO calculations