Rational Design of TiC-Supported Single-Atom Electrocatalysts for Hydrogen Evolution and Selective Oxygen Reduction Reactions

Abstract

We use a combination of density functional theory (DFT) calculations and experimental approaches to explore the stability and electrocatalytic activity of a wide range of transitionmetal single atoms on a TiC support. Our theoretical prediction that single atoms can be stabilized on the modified TiC surface is confirmed by experimental findings using them on a TiC support. The predicted activities where Pt and Au single atoms would be the best for hydrogen evolution and selective oxygen reduction reactions, respectively, agree well with experimental results. This rational strategy using computational modeling of materials enables effective design of highly active and stable single-atom catalysts.

Palladium Single‐Atom Catalysts Supported on C@C3N4 for Electrochemical Reactions

“…However, C@C 3 N 4 ‐0.5 %Pt showed much higher Tafel slope of 67 mV dec −1 , indicating that Heyrovsky step (H*+H 3 O + +e − →H 2 (g)+H 2 O) is RDS. This observation is consistent with other Pt single atom catalysts reported previously . The lack of Pt ensemble sites prevented re‐combination of adjacent H atoms, following Eley‐Rideal type of surface reaction.…”

“…This observation is consistent with other Pt single atom catalysts reported previously. [21] The lack of Pt ensemble sites prevented recombination of adjacent H atoms, following Eley-Rideal type of surface reaction.…”

Densely Populated Single Atom Catalysts

“…The as‐prepared FeSA‐G showed an ORR performance similar to that of Pt/C but with a higher stability. Moreover, these nano structure substrates with high specific surface area have additional advantages: 1) It can maximize the accessibility of the high‐density single atom active sites on the exposed high area support surface; 2) Single atomic sites can be clearly characterized on simple ordered low‐dimensional structures, such as graphene, MoS 2 , and MXene, etc . Typically, to robustly immobilize the metal atoms on the support, the heteroatoms doping, defects, and vacancies are usually introduced into the support to form strong interaction with metal atoms.…”

Unraveling the single-atom electrocatalytic activity of transition metal-doped phosphorene

“…The interdependency between intermediate adsorption energies is analyzed via scaling relations is shown in Figure 4 which have been identified to be as pivotal factors in determining the electrocatalytic activity. [14][15][16][17] To identify the chemical origin of breaking of scaling relations, we have carried out a projected crystal Hamilton population analysis (pCOHP) for all the intermediates, which has recently verified to be an important activity descriptor for computational screening studies ( Figure 5). 39 The bonding 11 population is represented in the right and antibonding population represented in left respectively.…”