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

Talib, Shamraiz Hussain1,2; Bashir, Beenish3; Khan, Muhammad Ajmal3; Ali, Babar4; Mohamed, Sharmarke1,2; Qurashi, Ahsanulhaq1,2; Li, Jun5,6,7,8

2024-04-01

10.1002/eem2.12723

ENERGY & ENVIRONMENTAL MATERIALS   影响因子和分区

2575-0356

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 = Sc-1, Ti-1, V-1, Cr-1, Mn-1, Fe-1, Co-1, Ni-1, Cu-1, Zr-1, Nb-1, Mo-1, Ru-1, Rh-1, Pd-1, Ag-1, W-1, Re-1, Os-1, Ir-1, Pt-1, and Au-1) 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, Sc-1, Co-1, Fe-1, and Au-1/GY demonstrate promising catalytic efficiency in the HER due to idealistic Delta G(H*) values via the Volmer-Heyrovsky pathway. Notably, Sc-1 and Au-1/GY exhibit superior HER catalytic activity compared to other studied catalysts. Co-1/GY catalyst exhibits higher selectivity and activity for the OER, with an overpotential (0.46 V) comparable to MoC2, IrO2, and RuO2. Also, Rh-1 and Co-1/GY SACs exhibited promising electrocatalysts for the ORR, with an overpotential of 0.36 and 0.46 V, respectively. Therefore, Co-1/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 Co-1 and Rh-1 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.

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

SCI ; EI

英语

通讯

National Natural Science Foundation of China[22033005] ; National Key RD Project["2022YFA1503900","2022YFA1503000"] ; Guangdong Provincial Key Laboratory of Catalysis[2020B121201002]

Materials Science

Materials Science, Multidisciplinary

WOS:001198116900001

WILEY

20241515874441

Atoms ; Catalyst activity ; Catalyst selectivity ; Electrocatalysts ; Electrolysis ; Electrolytic reduction ; Free energy ; Gibbs free energy ; Hydrogen ; Molecular dynamics ; Potential energy ; Quantum chemistry ; Reaction kinetics ; Ruthenium compounds ; Transition metals

Metallurgy and Metallography:531 ; Ore Treatment:533.1 ; Thermodynamics:641.1 ; Physical Chemistry:801.4 ; Electrochemistry:801.4.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Atomic and Molecular Physics:931.3

Web of Science

1.Khalifa Univ Sci & Technol, Adv Mat Chem Ctr AMCC, POB 127788, Abu Dhabi, U Arab Emirates
2.Khalifa Univ Sci & Technol, Dept Chem, POB 127788, Abu Dhabi, U Arab Emirates
3.George Mason Univ, Dept Chem & Biochem, 4400 Univ Dr, Fairfax, VA 22030 USA
4.King Fahd Univ Petr & Minerals, Interdisciplinary Res Ctr Refining & Adv Chem, Dhahran 31261, Saudi Arabia
5.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
6.Tsinghua Univ, Engn Res Ctr Adv Rare Earth Mat, Minist Educ, Beijing 100084, Peoples R China
7.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China
8.Southern Univ Sci & Technol, Guangdong Prov Key Lab Catalyt Chem, Shenzhen 518055, Peoples R China

Talib, Shamraiz Hussain,Bashir, Beenish,Khan, Muhammad Ajmal,et al. Improving the Efficiency of Water Splitting and Oxygen Reduction Via Single-Atom Anchoring on Graphyne Support[J]. ENERGY & ENVIRONMENTAL MATERIALS,2024,7.

Talib, Shamraiz Hussain.,Bashir, Beenish.,Khan, Muhammad Ajmal.,Ali, Babar.,Mohamed, Sharmarke.,...&Li, Jun.(2024).Improving the Efficiency of Water Splitting and Oxygen Reduction Via Single-Atom Anchoring on Graphyne Support.ENERGY & ENVIRONMENTAL MATERIALS,7.

Talib, Shamraiz Hussain,et al."Improving the Efficiency of Water Splitting and Oxygen Reduction Via Single-Atom Anchoring on Graphyne Support".ENERGY & ENVIRONMENTAL MATERIALS 7(2024).