Electrochemical CO₂Reduction over Metal-/Nitrogen-Doped Graphene Single-Atom Catalysts Modeled Using the Grand-Canonical Density Functional Theory

Renewably driven, electrochemical conversion of carbon dioxide into value-added products is expected to be a critical tool in global decarbonization. However, theoretical studies based on the computational hydrogen electrode largely ignore the nonlinear effects of the applied potential on the calculated results, leading to inaccurate...

Breaking Linear Scaling Relationships with Secondary Interactions in Confined Space: A Case Study of Methane Oxidation by Fe/ZSM-5 Zeolite

Linear energy scaling laws connect the kinetic and thermodynamic parameters of key elementary steps for heterogeneously catalyzed reactions over defined active sites on open surfaces. Such scaling laws provide a framework for a rapid computational activity screening of families of catalysts, but they also effectively impose a fundamental...

Computational insights into the catalytic role of the base promoters in ester hydrogenation with homogeneous non-pincer-based Mn-P,N catalyst

The reaction mechanism of ester hydrogenation catalyzed by a bidentate aminophosphine ligated manganese catalyst was studied by DFT calculations. Particular emphasize was placed on the role of the alkoxide base additives. The presence of such basic promoters as KO^tBu can improve the catalyst activity by lowering the activation...

An Active Alkali-Exchanged Faujasite Catalyst for p-Xylene Production via the One-Pot Diels-Alder Cycloaddition/Dehydration Reaction of 2,5-Dimethylfuran with Ethylene

The one-pot Diels-Alder cycloaddition (DAC)/dehydration (D) tandem reaction between 2,5-dimethylfuran and ethylene is a potent pathway toward biomass-derived p-xylene. In this work, we present a cheap and active low-silica potassium-exchanged faujasite (KY, Si/Al = 2.6) catalyst. Catalyst optimization was guided by a computational study of...

The electrochemical sodiation of sb investigated by Operando X-ray absorption and ¹²¹ sb mössbauer spectroscopy: What does one really learn?

In this study, we want to highlight the assets and restrictions of X-ray absorption spectroscopy (XAS) and Mössbauer spectroscopy for investigating the mechanism of the electrochemical reaction of antimony electrode materials vs. Na. For this, operando XAS was carried out during the first one and a half cycles, and the whole set of measured...

Organic crystals and improved electrolyte for aqueous sodium-ion batteries: Fundamental insights in new organic anode materials for aqueous sodium-ion batteries using DFT calculations and experimental insights in increased electrolyte stability

Density Functional Theory (DFT) calculations were performed to explore the electrochemical properties of two organic molecules that show promise to serve as affordable and safe anode materials in aqueous sodium-ion batteries. Upon sodium insertion, N,N’ –bis(methyl)- 1,4,5,8-naphthalene diimide (NDMe) appears to share sodium atoms with three...

Probing the local environment of a single OPE3 molecule using inelastic tunneling electron spectroscopy

We study single-molecule oligo(phenylene ethynylene)dithiol junctions by means of inelastic electron tunneling spectroscopy (IETS). The molecule is contacted with gold nano-electrodes formed with the mechanically controllable break junction technique. We record the IETS spectrum of the molecule from direct current measurements, both as a...