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Title: Assessing Carbon-Based Anodes for Lithium-Ion Batteries: A Universal Description of Charge-Transfer Binding

Many key performance characteristics of carbon-based lithium-ion battery anodes are largely determined by the strength of binding between lithium (Li) and sp2 carbon (C), which can vary significantly with subtle changes in substrate structure, chemistry, and morphology. We use density functional theory calculations to investigate the interactions of Li with a wide variety of sp2 C substrates, including pristine, defective, and strained graphene, planar C clusters, nanotubes, C edges, and multilayer stacks. In almost all cases, we find a universal linear relation between the Li-C binding energy and the work required to fill previously unoccupied electronic states within the substrate. This suggests that Li capacity is predominantly determined by two key factors—namely, intrinsic quantum capacitance limitations and the absolute placement of the Fermi level. This simple descriptor allows for straightforward prediction of the Li-C binding energy and related battery characteristics in candidate C materials based solely on the substrate electronic structure. It further suggests specific guidelines for designing more effective C-based anodes. Furthermore, this method should be broadly applicable to charge-transfer adsorption on planar substrates, and provides a phenomenological connection to established principles in supercapacitor and catalyst design.
Authors:
 [1] ;  [2] ;  [1] ;  [3]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Quantum Simulations Group; Rice Univ., Houston, TX (United States). Dept. of Materials Science and NanoEngineering, Chemistry, and Smalley Inst. for Nanoscale Science and Technology
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Nanoscale Synthesis and Characterization Lab.
  3. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Quantum Simulations Group
Publication Date:
OSTI Identifier:
1325867
Report Number(s):
LLNL-JRNL--652098
Journal ID: ISSN 0031-9007; PRLTAO
Grant/Contract Number:
AC52-07NA27344
Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 113; Journal Issue: 2; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Research Org:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 25 ENERGY STORAGE