Lithium Diffusion in Graphitic Carbon Kristin Persson Vijay A. Sethuraman Laurence J. Hardwick Yoyo Hinuma Ying Shirley Meng Anton van der Ven Venkat Srinivasan Robert Kostecki Gerbrand Ceder 10.1021/jz100188d.s001 https://acs.figshare.com/articles/journal_contribution/Lithium_Diffusion_in_Graphitic_Carbon/2012844 Graphitic carbon is currently considered the state-of-the-art material for the negative electrode in lithium ion cells, mainly due to its high reversibility and low operating potential. However, carbon anodes exhibit mediocre charge/discharge rate performance, which contributes to severe transport-induced surface structural damage upon prolonged cycling and limits the lifetime of the cell. Lithium bulk diffusion in graphitic carbon is not yet completely understood, partly due to the complexity of measuring bulk transport properties in finite-sized nonisotropic particles. To solve this problem for graphite, we use the Devanathan−Stachurski electrochemical methodology combined with ab initio computations to deconvolute and quantify the mechanism of lithium ion diffusion in highly oriented pyrolytic graphite (HOPG). The results reveal inherent high lithium ion diffusivity in the direction parallel to the graphene plane (∼10<sup>−7</sup>−10<sup>−6</sup> cm<sup>2</sup> s<sup>−1</sup>), as compared to sluggish lithium ion transport along grain boundaries (∼10<sup>−11</sup> cm<sup>2</sup> s<sup>−1</sup>), indicating the possibility of rational design of carbonaceous materials and composite electrodes with very high rate capability. 2015-12-16 16:36:54 cm pyrolytic graphite lithium ion diffusion bulk transport properties electrode carbonaceous materials Lithium Diffusion Graphitic CarbonGraphitic carbon carbon anodes exhibit graphitic carbon Lithium bulk diffusion lithium ion transport ab initio computations rate capability lithium ion diffusivity lithium ion cells HOPG