Examining the rudimentary steps of the oxygen reduction reaction on single-atomic Pt using Ti-based non-oxide supports

Tak, Young Joo; Yang, Sungeun; Lee, Hyunjoo; Lim, Dong‐Hee; Soon, Aloysius

doi:10.1016/j.jiec.2017.09.027

Cited by 15 publications

(5 citation statements)

References 56 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Along the favorable pathway, the reduction of O 2 to * OOH is the rate-limiting step with the largest activation barrier of 0.38 eV on Au/p-BN-V N catalyst. This value of E act is smaller than that of the reported single Pt on TiC(111) catalysts ( E act = 0.51 eV) and pure Pt(111) surface ( E act = 0.79 eV) (Duan and Wang, 2011; Tak et al, 2018).…”

Section: Resultsmentioning

confidence: 56%

Isolated Au Atom Anchored on Porous Boron Nitride as a Promising Electrocatalyst for Oxygen Reduction Reaction (ORR): A DFT Study

Zhang

et al. 2019

Front. Chem.

View full text Add to dashboard Cite

The development of efficient, stable, and low-cost catalytic material for the oxygen reduction reaction (ORR) is currently highly desirable but challenging. In this work, based on first-principles calculation, the stabilities, catalytic activities and catalytic mechanisms of isolated Au atom supported on defective porous BN (p-BN) have been studied in detail. The results reveal that the defective p-BN anchor Au atom strongly to ensure the stability of Au/p-BN. Based on frontier molecular orbital and charge-density analysis, isolated Au atom supported on porous BN with VN defect (Au/p-BN-VN) is an effective ORR catalyst. Especially, the low barriers of the formation (0.38 eV) and dissociation (0.31 eV) of *OOH and the instability of H2O2 on Au/p-BN-VN catalyst suggest that ORR proceeds via 4-electron pathway. Along the favorable pathway, the reduction of O2 to *OOH is the rate-limiting step with the largest activation barrier of 0.38 eV and the maximum free energy change is 1.88 eV. Our results provide a useful guidance for the design and fabrication of new Au-base catalyst with high-efficiency and are beneficial for the developing of novel isolated metal atom catalysts for ORR.

show abstract

Section: Resultsmentioning

confidence: 56%

Isolated Au Atom Anchored on Porous Boron Nitride as a Promising Electrocatalyst for Oxygen Reduction Reaction (ORR): A DFT Study

Zhang

et al. 2019

Front. Chem.

View full text Add to dashboard Cite

show abstract

“…The active center is constructed by a single Pt atom adsorption for the ORR intermediates to adsorb and to react. Single-atom catalysis has been reported to provide a superior catalytic performance in many systems. − From the computational point of view, the single-atom catalyst represents a simplified, primary model that provides fundamental insights and explanation to the material properties, as is frequently constructed in many theoretical studies, − for example, single Pt atom catalysis for ORR on doped graphene. , Our detailed density of states (DOS) and Bader charge population analyses indicate a weaker bonding between the surfaces with the F terminators than those with O, and we observe a linear variation between the overall ORR performance and the O/F ratio. The free-energy diagrams as well as the volcano plots for the ORR intermediates are also computed.…”

Section: Introductionmentioning

confidence: 68%

Termination Effects of Pt/v-Ti_n+1C_nT₂ MXene Surfaces for Oxygen Reduction Reaction Catalysis

Liu

2018

ACS Appl. Mater. Interfaces

103

View full text Add to dashboard Cite

Ideal catalysts for the oxygen reduction reaction (ORR) have been searched and researched for decades with the goal to overcome the overpotential problem in proton exchange membrane fuel cells. A recent experimental study reports the application of Pt nanoparticles on the newly discovered 2D material, MXene, with high stability and good performance in ORR. In this work, we simulate the Ti n+1C n T x and the Pt-decorated Pt/v-Ti n+1C n T x (n = 1–3, T = O and/or F) surfaces by first-principles calculations. We focus on the termination effects of MXene, which may be an important factor to enhance the performance of ORR. The properties of different surfaces are clarified by exhaustive computational analyses on the geometries, charges, and their electronic structures. The free-energy diagrams as well as the volcano plots for ORR are also calculated. On the basis of our results, the F-terminated surfaces are predicted to show a better performance for ORR but with a lower stability than the O-terminated counterparts, and the underlying mechanisms are investigated in detail. This study provides a better understanding of the electronic effect induced by the terminators and may inspire realizations of practical MXene systems for ORR catalysis.

show abstract

“…The reaction free energy (Δ G ) of every elementary step during CO 2 ERR was calculated based on the computational hydrogen electrode (CHE) model . The Δ G value was calculated as Δ G = Δ E + ΔZPE – T Δ S , , where Δ E was the change of total energy, ΔZPE was the change of the zero-point energy, Δ S was the change of entropy, and T was the temperature and was set as 298.15 K . The conductor-like screening model (COSMO) was used to simulate the aqueous environment, and the dielectric constant was set to 78.54 …”

Section: Methodsmentioning

confidence: 99%

Metal-Doped Two-Dimensional Borophene Nanosheets for the Carbon Dioxide Electrochemical Reduction Reaction

Hou

et al. 2020

J. Phys. Chem. C

View full text Add to dashboard Cite

Electrochemical reduction of carbon dioxide into hydrocarbons can promote the carbon dioxide utilization and decrease the greenhouse effect. In this work, the electrochemical reduction of carbon dioxide on metal-doped α-borophene nanosheets was studied based on density functional theory. Our results show that the reduction of carbon dioxide on different metal-doped α-borophene nanosheets proceeds through different preferred pathway. The free energies of the rate-determining step increase in the order of Co- = Fe- < Pd- < Pt- < Ni- < Rh- < Ru- < Ir- < Os-doped α-borophene. A nearly linear relationship was observed between the reaction free energies of the rate-determining step and the adsorption energies of carbon dioxide on metal-doped α-borophene nanosheets. Furthermore, the reduction of carbon dioxide was energetically more favorable than the hydrogen evolution reaction on Co- and Pd-doped α-borophene nanosheets.

show abstract

Examining the rudimentary steps of the oxygen reduction reaction on single-atomic Pt using Ti-based non-oxide supports

Cited by 15 publications

References 56 publications

Isolated Au Atom Anchored on Porous Boron Nitride as a Promising Electrocatalyst for Oxygen Reduction Reaction (ORR): A DFT Study

Isolated Au Atom Anchored on Porous Boron Nitride as a Promising Electrocatalyst for Oxygen Reduction Reaction (ORR): A DFT Study

Termination Effects of Pt/v-Ti_n+1C_nT₂ MXene Surfaces for Oxygen Reduction Reaction Catalysis

Metal-Doped Two-Dimensional Borophene Nanosheets for the Carbon Dioxide Electrochemical Reduction Reaction

Contact Info

Product

Resources

About

Examining the rudimentary steps of the oxygen reduction reaction on single-atomic Pt using Ti-based non-oxide supports

Cited by 15 publications

References 56 publications

Isolated Au Atom Anchored on Porous Boron Nitride as a Promising Electrocatalyst for Oxygen Reduction Reaction (ORR): A DFT Study

Isolated Au Atom Anchored on Porous Boron Nitride as a Promising Electrocatalyst for Oxygen Reduction Reaction (ORR): A DFT Study

Termination Effects of Pt/v-Tin+1CnT2 MXene Surfaces for Oxygen Reduction Reaction Catalysis

Metal-Doped Two-Dimensional Borophene Nanosheets for the Carbon Dioxide Electrochemical Reduction Reaction

Contact Info

Product

Resources

About

Termination Effects of Pt/v-Ti_n+1C_nT₂ MXene Surfaces for Oxygen Reduction Reaction Catalysis