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

Chi You Liu, Elise Yu-Tzu Li

Research output: Contribution to journalArticle

1 Citation (Scopus)

Abstract

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 Tin+1CnTx and the Pt-decorated Pt/v-Tin+1CnTx (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.

Original languageEnglish
JournalACS Applied Materials and Interfaces
DOIs
Publication statusPublished - 2019 Jan 9

Fingerprint

Tin
Catalysis
Oxygen
Volcanoes
Proton exchange membrane fuel cells (PEMFC)
Free energy
Electronic structure
Nanoparticles
Catalysts
Geometry

Keywords

  • DFT
  • MXene
  • VASP
  • oxygen reduction reaction
  • single atom catalysis
  • termination effects

ASJC Scopus subject areas

  • Materials Science(all)

Cite this

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title = "Termination Effects of Pt/v-Tin+1CnT2 MXene Surfaces for Oxygen Reduction Reaction Catalysis",
abstract = "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 Tin+1CnTx and the Pt-decorated Pt/v-Tin+1CnTx (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.",
keywords = "DFT, MXene, VASP, oxygen reduction reaction, single atom catalysis, termination effects",
author = "Liu, {Chi You} and Li, {Elise Yu-Tzu}",
year = "2019",
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AU - Li, Elise Yu-Tzu

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N2 - 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 Tin+1CnTx and the Pt-decorated Pt/v-Tin+1CnTx (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.

AB - 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 Tin+1CnTx and the Pt-decorated Pt/v-Tin+1CnTx (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.

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