Li intercalation in graphite: a van der Waals density functional study

E. Hazrati, G.A. de Wijs, G. Brocks

Research output: Contribution to journalArticleAcademicpeer-review

32 Citations (Scopus)

Abstract

Modeling layered intercalation compounds from first principles poses a problem, as many of their properties are determined by a subtle balance between van der Waals interactions and chemical or Madelung terms, and a good description of van der Waals interactions is often lacking. Using van der Waals density functionals we study the structures, phonons and energetics of the archetype layered intercalation compound Li-graphite. Intercalation of Li in graphite leads to stable systems with calculated intercalation energies of −0.2 to −0.3 eV/Li atom, (referred to bulk graphite and Li metal). The fully loaded stage 1 and stage 2 compounds LiC 6 and Li 1/2 C 6 are stable, corresponding to two-dimensional 3 √ ×3 √ lattices of Li atoms intercalated between two graphene planes. Stage N>2 structures are unstable compared to dilute stage 2 compounds with the same concentration. At elevated temperatures dilute stage 2 compounds easily become disordered, but the structure of Li 3/16 C 6 is relatively stable, corresponding to a 7 √ ×7 √ in-plane packing of Li atoms. First-principles calculations, along with a Bethe-Peierls model of finite temperature effects, allow for a microscopic description of the observed voltage profiles
Original languageUndefined
Pages (from-to)155448/1-155448/11
Number of pages11
JournalPhysical review B: Condensed matter and materials physics
Volume90
DOIs
Publication statusPublished - 2014

Keywords

  • METIS-306415
  • IR-94962

Cite this

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title = "Li intercalation in graphite: a van der Waals density functional study",
abstract = "Modeling layered intercalation compounds from first principles poses a problem, as many of their properties are determined by a subtle balance between van der Waals interactions and chemical or Madelung terms, and a good description of van der Waals interactions is often lacking. Using van der Waals density functionals we study the structures, phonons and energetics of the archetype layered intercalation compound Li-graphite. Intercalation of Li in graphite leads to stable systems with calculated intercalation energies of −0.2 to −0.3 eV/Li atom, (referred to bulk graphite and Li metal). The fully loaded stage 1 and stage 2 compounds LiC 6 and Li 1/2 C 6 are stable, corresponding to two-dimensional 3 √ ×3 √ lattices of Li atoms intercalated between two graphene planes. Stage N>2 structures are unstable compared to dilute stage 2 compounds with the same concentration. At elevated temperatures dilute stage 2 compounds easily become disordered, but the structure of Li 3/16 C 6 is relatively stable, corresponding to a 7 √ ×7 √ in-plane packing of Li atoms. First-principles calculations, along with a Bethe-Peierls model of finite temperature effects, allow for a microscopic description of the observed voltage profiles",
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Li intercalation in graphite: a van der Waals density functional study. / Hazrati, E.; de Wijs, G.A.; Brocks, G.

In: Physical review B: Condensed matter and materials physics, Vol. 90, 2014, p. 155448/1-155448/11.

Research output: Contribution to journalArticleAcademicpeer-review

TY - JOUR

T1 - Li intercalation in graphite: a van der Waals density functional study

AU - Hazrati, E.

AU - de Wijs, G.A.

AU - Brocks, G.

PY - 2014

Y1 - 2014

N2 - Modeling layered intercalation compounds from first principles poses a problem, as many of their properties are determined by a subtle balance between van der Waals interactions and chemical or Madelung terms, and a good description of van der Waals interactions is often lacking. Using van der Waals density functionals we study the structures, phonons and energetics of the archetype layered intercalation compound Li-graphite. Intercalation of Li in graphite leads to stable systems with calculated intercalation energies of −0.2 to −0.3 eV/Li atom, (referred to bulk graphite and Li metal). The fully loaded stage 1 and stage 2 compounds LiC 6 and Li 1/2 C 6 are stable, corresponding to two-dimensional 3 √ ×3 √ lattices of Li atoms intercalated between two graphene planes. Stage N>2 structures are unstable compared to dilute stage 2 compounds with the same concentration. At elevated temperatures dilute stage 2 compounds easily become disordered, but the structure of Li 3/16 C 6 is relatively stable, corresponding to a 7 √ ×7 √ in-plane packing of Li atoms. First-principles calculations, along with a Bethe-Peierls model of finite temperature effects, allow for a microscopic description of the observed voltage profiles

AB - Modeling layered intercalation compounds from first principles poses a problem, as many of their properties are determined by a subtle balance between van der Waals interactions and chemical or Madelung terms, and a good description of van der Waals interactions is often lacking. Using van der Waals density functionals we study the structures, phonons and energetics of the archetype layered intercalation compound Li-graphite. Intercalation of Li in graphite leads to stable systems with calculated intercalation energies of −0.2 to −0.3 eV/Li atom, (referred to bulk graphite and Li metal). The fully loaded stage 1 and stage 2 compounds LiC 6 and Li 1/2 C 6 are stable, corresponding to two-dimensional 3 √ ×3 √ lattices of Li atoms intercalated between two graphene planes. Stage N>2 structures are unstable compared to dilute stage 2 compounds with the same concentration. At elevated temperatures dilute stage 2 compounds easily become disordered, but the structure of Li 3/16 C 6 is relatively stable, corresponding to a 7 √ ×7 √ in-plane packing of Li atoms. First-principles calculations, along with a Bethe-Peierls model of finite temperature effects, allow for a microscopic description of the observed voltage profiles

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