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Title: Boosting the Low-Temperature Performance of Graphite Anodes by Creating an Electrochemically Active Interface

Journal Article · · ACS Applied Energy Materials
ORCiD logo [1];  [2]; ORCiD logo [3];  [4]; ORCiD logo [4]; ORCiD logo [2]
  1. Indiana University-Purdue University Indianapolis (IUPUI), Indianapolis, IN (United States); Purdue University, West Lafayette, IN (United States)
  2. Indiana University-Purdue University Indianapolis (IUPUI), Indianapolis, IN (United States)
  3. Argonne National Laboratory (ANL), Argonne, IL (United States)
  4. University of Pennsylvania, Philadelphia, PA (United States)

Graphite is the major anode material used in commercial lithium-ion batteries (LIBs). However, the sluggish ion-transfer kinetics associated with graphite anodes significantly restrict the operation of LIBs over a wide temperature. This is primarily due to their low reversible capacity and the substantial overpotential exhibited under low-temperature conditions. To address this limitation, we demonstrate herein an approach that involves grafting an electrochemically active lithium benzenesulfonate layer onto a graphite surface through a typical reduction reaction of diazonium cations, followed by ion exchange process. This surface modification reduces the charge transfer resistance of graphite anodes, leading to an excellent reversible capacity of ~150 mAh g–1 at low-temperatures (-20 °C, 0.1C). Electrochemical impedance spectroscopy indicates that both desolvation of the lithium ions outside the graphite, and lithium diffusion within the solid electrolyte interphase and graphite lattice are two crucial rate-limiting steps during the Li (de)lithiation, with the latter dominating during the low-temperature operation. In conclusion, these findings demonstrate a facile method for enhancing the low-temperature performance of graphite through surface modification and provide valuable insights into fundamental understandings that can guide the future design of better -low-temperature graphite anodes.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
Indiana University/Purdue University at Indianapolis (IUPUI); National Science Foundation (NSF); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
2484288
Journal Information:
ACS Applied Energy Materials, Journal Name: ACS Applied Energy Materials Journal Issue: 24 Vol. 6; ISSN 2574-0962
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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