Improving the Efficiency of Water Splitting and Oxygen Reduction Via Single-Atom Anchoring on Graphyne Support

Shamraiz Hussain Talib; Beenish Bashir; Muhammad Ajmal Khan; Babar Ali; Sharmarke Mohamed; Ahsanulhaq Qurashi; Jun Li

doi:10.1002/eem2.12723

Improving the Efficiency of Water Splitting and Oxygen Reduction Via Single-Atom Anchoring on Graphyne Support

Shamraiz Hussain Talib, Beenish Bashir, Muhammad Ajmal Khan, Babar Ali, Sharmarke Mohamed^*, Ahsanulhaq Qurashi^*, Jun Li^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

4 Scopus citations

Abstract

Single-atom catalysts (SACs) have received significant interest for optimizing metal atom utilization and superior catalytic performance in hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR). In this study, we investigate a range of single-transition metal (STM₁ = Sc₁, Ti₁, V₁, Cr₁, Mn₁, Fe₁, Co₁, Ni₁, Cu₁, Zr₁, Nb₁, Mo₁, Ru₁, Rh₁, Pd₁, Ag₁, W₁, Re₁, Os₁, Ir₁, Pt₁, and Au₁) atoms supported on graphyne (GY) surface for HER/OER and ORR using first-principle calculations. Ab initio molecular dynamics (AIMD) simulations and phonon dispersion spectra reveal the dynamic and thermal stabilities of the GY surface. The exceptional stability of all supported STM₁ atoms within the H1 cavity of the GY surface exists in an isolated form, facilitating the uniform distribution and proper arrangement of single atoms on GY. In particular, Sc₁, Co₁, Fe₁, and Au₁/GY demonstrate promising catalytic efficiency in the HER due to idealistic ΔG_H* values via the Volmer-Heyrovsky pathway. Notably, Sc₁ and Au₁/GY exhibit superior HER catalytic activity compared to other studied catalysts. Co₁/GY catalyst exhibits higher selectivity and activity for the OER, with an overpotential (0.46 V) comparable to MoC₂, IrO₂, and RuO₂. Also, Rh₁ and Co₁/GY SACs exhibited promising electrocatalysts for the ORR, with an overpotential of 0.36 and 0.46 V, respectively. Therefore, Co₁/GY is a versatile electrocatalyst for metal-air batteries and water-splitting. This study further incorporates computational analysis of the kinetic potential energy barriers of Co₁ and Rh₁ in the OER and ORR. A strong correlation is found between the estimated kinetic activation barriers for the thermodynamic outcomes and all proton-coupled electron transfer steps. We establish a relation for the Gibbs free energy of intermediates to understand the mechanism of SACs supported on STM₁/GY and introduce a key descriptor. This study highlights GY as a favorable single-atom support for designing highly active and cost-effective versatile electrocatalysts for practical applications.

Original language	English
Article number	e12723
Journal	Energy and Environmental Materials
Volume	7
Issue number	5
DOIs	https://doi.org/10.1002/eem2.12723
State	Accepted/In press - 2024

Bibliographical note

Publisher Copyright:
© 2024 The Authors. Energy & Environmental Materials published by John Wiley & Sons Australia, Ltd on behalf of Zhengzhou University.

Keywords

Graphyne Support
Hydrogen Evolution Reaction
Oxygen Evolution Reaction
Oxygen Reduction Reaction
Single-Atom Catalyst
Water Splitting

ASJC Scopus subject areas

Renewable Energy, Sustainability and the Environment
General Materials Science
Water Science and Technology
Environmental Science (miscellaneous)
Waste Management and Disposal
Energy (miscellaneous)

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1002/eem2.12723

Cite this

@article{e01dc26ff1ff408e87ff0f0850a45c01,

title = "Improving the Efficiency of Water Splitting and Oxygen Reduction Via Single-Atom Anchoring on Graphyne Support",

abstract = "Single-atom catalysts (SACs) have received significant interest for optimizing metal atom utilization and superior catalytic performance in hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR). In this study, we investigate a range of single-transition metal (STM1 = Sc1, Ti1, V1, Cr1, Mn1, Fe1, Co1, Ni1, Cu1, Zr1, Nb1, Mo1, Ru1, Rh1, Pd1, Ag1, W1, Re1, Os1, Ir1, Pt1, and Au1) atoms supported on graphyne (GY) surface for HER/OER and ORR using first-principle calculations. Ab initio molecular dynamics (AIMD) simulations and phonon dispersion spectra reveal the dynamic and thermal stabilities of the GY surface. The exceptional stability of all supported STM1 atoms within the H1 cavity of the GY surface exists in an isolated form, facilitating the uniform distribution and proper arrangement of single atoms on GY. In particular, Sc1, Co1, Fe1, and Au1/GY demonstrate promising catalytic efficiency in the HER due to idealistic ΔGH* values via the Volmer-Heyrovsky pathway. Notably, Sc1 and Au1/GY exhibit superior HER catalytic activity compared to other studied catalysts. Co1/GY catalyst exhibits higher selectivity and activity for the OER, with an overpotential (0.46 V) comparable to MoC2, IrO2, and RuO2. Also, Rh1 and Co1/GY SACs exhibited promising electrocatalysts for the ORR, with an overpotential of 0.36 and 0.46 V, respectively. Therefore, Co1/GY is a versatile electrocatalyst for metal-air batteries and water-splitting. This study further incorporates computational analysis of the kinetic potential energy barriers of Co1 and Rh1 in the OER and ORR. A strong correlation is found between the estimated kinetic activation barriers for the thermodynamic outcomes and all proton-coupled electron transfer steps. We establish a relation for the Gibbs free energy of intermediates to understand the mechanism of SACs supported on STM1/GY and introduce a key descriptor. This study highlights GY as a favorable single-atom support for designing highly active and cost-effective versatile electrocatalysts for practical applications.",

keywords = "Graphyne Support, Hydrogen Evolution Reaction, Oxygen Evolution Reaction, Oxygen Reduction Reaction, Single-Atom Catalyst, Water Splitting",

author = "Talib, {Shamraiz Hussain} and Beenish Bashir and Khan, {Muhammad Ajmal} and Babar Ali and Sharmarke Mohamed and Ahsanulhaq Qurashi and Jun Li",

note = "Publisher Copyright: {\textcopyright} 2024 The Authors. Energy & Environmental Materials published by John Wiley & Sons Australia, Ltd on behalf of Zhengzhou University.",

year = "2024",

doi = "10.1002/eem2.12723",

language = "English",

volume = "7",

journal = "Energy and Environmental Materials",

issn = "2575-0348",

publisher = "John Wiley & Sons Inc.",

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T1 - Improving the Efficiency of Water Splitting and Oxygen Reduction Via Single-Atom Anchoring on Graphyne Support

AU - Talib, Shamraiz Hussain

AU - Bashir, Beenish

AU - Khan, Muhammad Ajmal

AU - Ali, Babar

AU - Mohamed, Sharmarke

AU - Qurashi, Ahsanulhaq

AU - Li, Jun

PY - 2024

Y1 - 2024

N2 - Single-atom catalysts (SACs) have received significant interest for optimizing metal atom utilization and superior catalytic performance in hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR). In this study, we investigate a range of single-transition metal (STM1 = Sc1, Ti1, V1, Cr1, Mn1, Fe1, Co1, Ni1, Cu1, Zr1, Nb1, Mo1, Ru1, Rh1, Pd1, Ag1, W1, Re1, Os1, Ir1, Pt1, and Au1) atoms supported on graphyne (GY) surface for HER/OER and ORR using first-principle calculations. Ab initio molecular dynamics (AIMD) simulations and phonon dispersion spectra reveal the dynamic and thermal stabilities of the GY surface. The exceptional stability of all supported STM1 atoms within the H1 cavity of the GY surface exists in an isolated form, facilitating the uniform distribution and proper arrangement of single atoms on GY. In particular, Sc1, Co1, Fe1, and Au1/GY demonstrate promising catalytic efficiency in the HER due to idealistic ΔGH* values via the Volmer-Heyrovsky pathway. Notably, Sc1 and Au1/GY exhibit superior HER catalytic activity compared to other studied catalysts. Co1/GY catalyst exhibits higher selectivity and activity for the OER, with an overpotential (0.46 V) comparable to MoC2, IrO2, and RuO2. Also, Rh1 and Co1/GY SACs exhibited promising electrocatalysts for the ORR, with an overpotential of 0.36 and 0.46 V, respectively. Therefore, Co1/GY is a versatile electrocatalyst for metal-air batteries and water-splitting. This study further incorporates computational analysis of the kinetic potential energy barriers of Co1 and Rh1 in the OER and ORR. A strong correlation is found between the estimated kinetic activation barriers for the thermodynamic outcomes and all proton-coupled electron transfer steps. We establish a relation for the Gibbs free energy of intermediates to understand the mechanism of SACs supported on STM1/GY and introduce a key descriptor. This study highlights GY as a favorable single-atom support for designing highly active and cost-effective versatile electrocatalysts for practical applications.

AB - Single-atom catalysts (SACs) have received significant interest for optimizing metal atom utilization and superior catalytic performance in hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR). In this study, we investigate a range of single-transition metal (STM1 = Sc1, Ti1, V1, Cr1, Mn1, Fe1, Co1, Ni1, Cu1, Zr1, Nb1, Mo1, Ru1, Rh1, Pd1, Ag1, W1, Re1, Os1, Ir1, Pt1, and Au1) atoms supported on graphyne (GY) surface for HER/OER and ORR using first-principle calculations. Ab initio molecular dynamics (AIMD) simulations and phonon dispersion spectra reveal the dynamic and thermal stabilities of the GY surface. The exceptional stability of all supported STM1 atoms within the H1 cavity of the GY surface exists in an isolated form, facilitating the uniform distribution and proper arrangement of single atoms on GY. In particular, Sc1, Co1, Fe1, and Au1/GY demonstrate promising catalytic efficiency in the HER due to idealistic ΔGH* values via the Volmer-Heyrovsky pathway. Notably, Sc1 and Au1/GY exhibit superior HER catalytic activity compared to other studied catalysts. Co1/GY catalyst exhibits higher selectivity and activity for the OER, with an overpotential (0.46 V) comparable to MoC2, IrO2, and RuO2. Also, Rh1 and Co1/GY SACs exhibited promising electrocatalysts for the ORR, with an overpotential of 0.36 and 0.46 V, respectively. Therefore, Co1/GY is a versatile electrocatalyst for metal-air batteries and water-splitting. This study further incorporates computational analysis of the kinetic potential energy barriers of Co1 and Rh1 in the OER and ORR. A strong correlation is found between the estimated kinetic activation barriers for the thermodynamic outcomes and all proton-coupled electron transfer steps. We establish a relation for the Gibbs free energy of intermediates to understand the mechanism of SACs supported on STM1/GY and introduce a key descriptor. This study highlights GY as a favorable single-atom support for designing highly active and cost-effective versatile electrocatalysts for practical applications.

KW - Graphyne Support

KW - Hydrogen Evolution Reaction

KW - Oxygen Evolution Reaction

KW - Oxygen Reduction Reaction

KW - Single-Atom Catalyst

KW - Water Splitting

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DO - 10.1002/eem2.12723

M3 - Article

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SN - 2575-0348

VL - 7

JO - Energy and Environmental Materials

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Improving the Efficiency of Water Splitting and Oxygen Reduction Via Single-Atom Anchoring on Graphyne Support

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

UN SDGs

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