Reaction mechanism and kinetics for carbon dioxide reduction on iron–nickel Bi-atom catalysts

Abstract

Electrochemical CO2 reduction reaction (CO2RR) is being accepted as one of the most promising strategy to convert carbon emissions to valuable chemicals and fuels. Among the various types of electrocatalysts,...

Reaction mechanism and kinetics of oxygen reduction reaction on the iron–nickel dual atom catalyst

“…37 To describe the explicit polarization effect involved in proton transfer events, we added three explicit water molecules in a vertical direction to the reaction system and performed the structural relaxation in VASPsol with a default dielectric constant of 3 = 78.4 for water. [32][33][34] It is worth mentioning that introducing only three explicit water molecules into the systems in the vertical direction, might not fully describe the inuence of the dynamic hydrogen bond network and might have some impacts on the calculated reaction barriers. In fact, the hydrogen dynamic transfer can also happen between more than three water molecules in other directions.…”

“…That is, we need to calculate the reaction barriers, reaction rates, charge transfer, and spin population of active metal site along the proton transfer steps that give rise to the current-potential (I-V) curves, Tafel slopes, and the concentration of each reaction intermediate on the catalyst's surface. [34][35][36] In addition, investigation of partial density of states along the proton transfer steps is needed to understand the changes in molecular orbital congurations responsible for the evolution in bonding interactions and Gibbs free energies. These aspects have been investigated partially for several electrochemical reactions on various catalysts.…”

“…That is, we need to calculate the reaction barriers, reaction rates, charge transfer, and spin population of active metal site along the proton transfer steps that give rise to the current–potential ( I – V ) curves, Tafel slopes, and the concentration of each reaction intermediate on the catalyst's surface. 34–36…”

Direct coupling of two inert CO2 molecules to form a C–C bond on the Cu0 atomic interfaces of the nitrogen-doped graphene-supported Cu4 cluster

“…[32][33][34][35][36][37] Especially in the study of M-N-C catalysts based on metal elements such as Cu, Ni, Fe, and Co, etc., it has been demonstrated that these catalysts have high activity and selectivity for the reduction of CO 2 to CO. [38][39][40][41][42] Among the various reported metals, the carbon-loaded Cu-based catalyst shows high activity in CO 2 RR. [43][44][45][46] These reported catalysts are of particular interest because of their ability to generate large amounts of hydrocarbons, including HCOOH, CH 4 , C 2 H 4 , etc. [47][48][49][50][51] Shen and co-workers found that the anchoring of Cu atoms on defective diamond graphene results in excellent catalytic performance for the selective conversion of acetylene to ethylene.…”

A Combined Reaction Path Search and Hybrid Solvation Method for the Systematic Exploration of Elementary Reactions at the Solid–Liquid Interface

“…To take account of the solvation effects in the chemical reaction at the solid–liquid interface, a hybrid simulation method combining the density functional theory (DFT) with the implicit solvation theory is one of the possible approaches to calculate the electronic structure for solvated systems. − Although the accuracy and computational time of the hybrid simulation method depend on the implicit solution theory, it enables us to determine the thermally averaged properties with one-shot calculation. Recently, the effective screening method combined with the reference interaction site model (ESM-RISM) has been developed for simulating the solid–liquid interface problems. , In ESM-RISM, the target system, e.g., an electrode surface with reactant molecule, is explicitly treated by DFT , with the ESM technique, and the solvation system is implicitly treated by RISM, , where the interaction between the explicit and implicit systems is described by the sum of electrostatic and van der Waals potentials.…”