Insights into the hydrogen dissociation mechanism on lithium edge-decorated carbon rings and graphene nanoribbon

Alejandro Vásquez-Espinal, Ricardo Pino-Rios, Patricio Fuentealba, Walter Orellana, William Tiznado

Resultado de la investigación: Article

8 Citas (Scopus)

Resumen

The purpose of this study is to show that H2 is easily dissociated on lithium edge decorated carbon systems to form strong C-H and Li-H bonds. This mechanism has not been considered in previous studies where these kinds of systems have been proposed as good candidates to serve as hydrogen storage materials. The reactivity of molecular hydrogen (H2) on three representative lithium edge-decorated carbon systems (on the clusters C5Li7 + (1) and C6Li6 (2), and on lithium edge-decorated zig-zag graphene nanoribbon (GNR-Li) (3)) have been studied using ab initio calculations based on the density functional theory with dispersion-corrected van der Waals exchange correlation functional. Our calculations show, on the one hand, that heterolytic hydrogen dissociation can precede with relatively low reaction barriers (0.60, 0.45 and 0.56 eV for systems 1, 2 and 3, respectively) along the minimum energy path and, on the other hand, that chemisorption energies are highly stabilizing (in the range of 1.15-1.54 eV). It is important to note that the highest activation barrier is found for the unique system, characterized as global minimum, on its corresponding potential energy surface (PES), which is system 1. These findings suggest that reversibility of the hydrogen absorption/desorption reactions, required in promising hydrogen storage materials, does not apply in these systems.

Idioma originalEnglish
PublicaciónInternational Journal of Hydrogen Energy
DOI
EstadoAccepted/In press - 25 nov 2015

Huella dactilar

Nanoribbons
Graphene
graphene
Lithium
lithium
Hydrogen storage
dissociation
Hydrogen
Carbon
carbon
rings
hydrogen
Potential energy surfaces
Chemisorption
Density functional theory
Desorption
Chemical activation
chemisorption
reactivity
desorption

ASJC Scopus subject areas

  • Renewable Energy, Sustainability and the Environment
  • Fuel Technology
  • Condensed Matter Physics
  • Energy Engineering and Power Technology

Citar esto

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title = "Insights into the hydrogen dissociation mechanism on lithium edge-decorated carbon rings and graphene nanoribbon",
abstract = "The purpose of this study is to show that H2 is easily dissociated on lithium edge decorated carbon systems to form strong C-H and Li-H bonds. This mechanism has not been considered in previous studies where these kinds of systems have been proposed as good candidates to serve as hydrogen storage materials. The reactivity of molecular hydrogen (H2) on three representative lithium edge-decorated carbon systems (on the clusters C5Li7 + (1) and C6Li6 (2), and on lithium edge-decorated zig-zag graphene nanoribbon (GNR-Li) (3)) have been studied using ab initio calculations based on the density functional theory with dispersion-corrected van der Waals exchange correlation functional. Our calculations show, on the one hand, that heterolytic hydrogen dissociation can precede with relatively low reaction barriers (0.60, 0.45 and 0.56 eV for systems 1, 2 and 3, respectively) along the minimum energy path and, on the other hand, that chemisorption energies are highly stabilizing (in the range of 1.15-1.54 eV). It is important to note that the highest activation barrier is found for the unique system, characterized as global minimum, on its corresponding potential energy surface (PES), which is system 1. These findings suggest that reversibility of the hydrogen absorption/desorption reactions, required in promising hydrogen storage materials, does not apply in these systems.",
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Insights into the hydrogen dissociation mechanism on lithium edge-decorated carbon rings and graphene nanoribbon. / Vásquez-Espinal, Alejandro; Pino-Rios, Ricardo; Fuentealba, Patricio; Orellana, Walter; Tiznado, William.

En: International Journal of Hydrogen Energy, 25.11.2015.

Resultado de la investigación: Article

TY - JOUR

T1 - Insights into the hydrogen dissociation mechanism on lithium edge-decorated carbon rings and graphene nanoribbon

AU - Vásquez-Espinal, Alejandro

AU - Pino-Rios, Ricardo

AU - Fuentealba, Patricio

AU - Orellana, Walter

AU - Tiznado, William

PY - 2015/11/25

Y1 - 2015/11/25

N2 - The purpose of this study is to show that H2 is easily dissociated on lithium edge decorated carbon systems to form strong C-H and Li-H bonds. This mechanism has not been considered in previous studies where these kinds of systems have been proposed as good candidates to serve as hydrogen storage materials. The reactivity of molecular hydrogen (H2) on three representative lithium edge-decorated carbon systems (on the clusters C5Li7 + (1) and C6Li6 (2), and on lithium edge-decorated zig-zag graphene nanoribbon (GNR-Li) (3)) have been studied using ab initio calculations based on the density functional theory with dispersion-corrected van der Waals exchange correlation functional. Our calculations show, on the one hand, that heterolytic hydrogen dissociation can precede with relatively low reaction barriers (0.60, 0.45 and 0.56 eV for systems 1, 2 and 3, respectively) along the minimum energy path and, on the other hand, that chemisorption energies are highly stabilizing (in the range of 1.15-1.54 eV). It is important to note that the highest activation barrier is found for the unique system, characterized as global minimum, on its corresponding potential energy surface (PES), which is system 1. These findings suggest that reversibility of the hydrogen absorption/desorption reactions, required in promising hydrogen storage materials, does not apply in these systems.

AB - The purpose of this study is to show that H2 is easily dissociated on lithium edge decorated carbon systems to form strong C-H and Li-H bonds. This mechanism has not been considered in previous studies where these kinds of systems have been proposed as good candidates to serve as hydrogen storage materials. The reactivity of molecular hydrogen (H2) on three representative lithium edge-decorated carbon systems (on the clusters C5Li7 + (1) and C6Li6 (2), and on lithium edge-decorated zig-zag graphene nanoribbon (GNR-Li) (3)) have been studied using ab initio calculations based on the density functional theory with dispersion-corrected van der Waals exchange correlation functional. Our calculations show, on the one hand, that heterolytic hydrogen dissociation can precede with relatively low reaction barriers (0.60, 0.45 and 0.56 eV for systems 1, 2 and 3, respectively) along the minimum energy path and, on the other hand, that chemisorption energies are highly stabilizing (in the range of 1.15-1.54 eV). It is important to note that the highest activation barrier is found for the unique system, characterized as global minimum, on its corresponding potential energy surface (PES), which is system 1. These findings suggest that reversibility of the hydrogen absorption/desorption reactions, required in promising hydrogen storage materials, does not apply in these systems.

KW - Ab initio calculations

KW - Carbon-lithium systems

KW - Hydrogen dissociation

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