First-principles analysis of defect-mediated Li adsorption on graphene

Handan Yildirim, Alper Kinaci, Zhi Jian Zhao, Maria K.Y. Chan, Jeffrey P. Greeley*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

120 Scopus citations


To evaluate the possible utility of single layer graphene for applications in Li ion batteries, an extensive series of periodic density functional theory (DFT) calculations are performed on graphene sheets with both point and extended defects for a wide range of lithium coverages. Consistent with recent reports, it is found that Li adsorption on defect-free single layer graphene is not thermodynamically favorable compared to bulk metallic Li. However, graphene surfaces activated by defects are generally found to bind Li more strongly, and the interaction strength is sensitive to both the nature of the defects and their densities. Double vacancy defects are found to have much stronger interactions with Li as compared to Stone-Wales defects, and increasing defect density also enhances the interaction of the Stone-Wales defects with Li. Li interaction with one-dimensional extended defects on graphene is additionally found to be strong and leads to increased Li adsorption. A rigorous thermodynamic analysis of these data establishes the theoretical Li storage capacities of the defected graphene structures. In some cases, these capacities are found to approach, although not exceed, those of graphite. The results provide new insights into the fundamental physics of adsorbate interactions with graphene defects and suggest that careful defect engineering of graphene might, ultimately, provide anode electrodes of suitable capacity for lithium ion battery applications.

Original languageEnglish (US)
Pages (from-to)21141-21150
Number of pages10
JournalACS Applied Materials and Interfaces
Issue number23
StatePublished - Dec 10 2014


  • defects
  • density functional theory
  • genetic algorithm
  • graphene
  • lithium ion battery
  • van der Waals interactions

ASJC Scopus subject areas

  • General Materials Science


Dive into the research topics of 'First-principles analysis of defect-mediated Li adsorption on graphene'. Together they form a unique fingerprint.

Cite this