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Title: Impact of Pore Tortuosity on Electrode Kinetics in Lithium Battery Electrodes: Study in Directionally Freeze-Cast LiNi0.8Co0.15Al0.05O2 (NCA)

Journal Article · · Journal of the Electrochemical Society
ORCiD logo [1];  [2];  [3];  [4];  [5];  [3]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering; Univ. of Mons (Belgium). Lab. of Physics of Surfaces and Interfaces
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Qatar Foundation, Doha (Qatar). Qatar Environment and Energy Research Inst.
  3. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering
  4. Univ. of Mons (Belgium). Lab. of Physics of Surfaces and Interfaces
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
+ Show Author Affiliations

The prevailing electrode fabrication method for lithium-ion battery electrodes includes calendering at high pressures to densify the electrode and promote adhesion to the metal current collector. However, this process increases the tortuosity of the pore network in the primary transport direction and imposes severe tradeoffs between electrode thickness and rate capability. With the aim of understanding the impact of pore tortuosity on electrode kinetics, and enabling cell designs with thicker electrodes and improved cost and energy density, we use here freeze-casting, a shaping technique able to produce low-tortuosity structures using ice crystals as a pore-forming agent, to fabricate LiNi0.8Co0.15Al0.05O2 (NCA) cathodes with controlled, aligned porosity. Electrode tortuosity is characterized using two complementary methods, X-ray tomography combined with thermal diffusion simulations, and electrochemical transport measurements. The results allow comparison across a wide range of microstructures, and highlight the large impact of a relatively small numerical change in tortuosity on electrode kinetics. Under galvanostatic discharge, optimized microstructures show a three- to fourfold increase in area-specific capacity compared to typical Li-ion composite electrodes. Hybrid pulse power characterization (HPPC) demonstrates improved power capability, while dynamic stress tests (DST) shows that an area-specific area capacity corresponding to 91% of the NCA galvanostatic C/10 capacity could be reached.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES); Belgian Science Policy Office; Région Wallone (Belgium); Wallonie-Bruxelles International (Belgium); National Fund for Scientific Research (FNRS) (Belgium); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1419826
Alternate ID(s):
OSTI ID: 1494080
Journal Information:
Journal of the Electrochemical Society, Vol. 165, Issue 2; ISSN 0013-4651
Publisher:
The Electrochemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 85 works
Citation information provided by
Web of Science

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Cited By (10)

Strategies for Building Robust Traffic Networks in Advanced Energy Storage Devices: A Focus on Composite Electrodes journal December 2018
Diffusion‐Limited C‐Rate: A Fundamental Principle Quantifying the Intrinsic Limits of Li‐Ion Batteries journal November 2019
High‐Voltage Performance of Ni‐Rich NCA Cathodes: Linking Operating Voltage with Cathode Degradation journal August 2019
Synthesis and electrochemical characterization of Cr-doped lithium-rich Li1.2Ni0.16Mn0.56Co0.08-xCrxO2 cathodes journal October 2018
Requirements for Enabling Extreme Fast Charging of High Energy Density Li-Ion Cells while Avoiding Lithium Plating journal January 2019
High-rate lithium ion energy storage to facilitate increased penetration of photovoltaic systems in electricity grids journal January 2019
Production and Characterization of a Silica-Alumina Membrane Using Novel Tubular Freeze-Cast Substrates journal January 2019
High-rate lithium ion energy storage to facilitate increased penetration of photovoltaic systems in electricity grids text January 2019
High-rate lithium ion energy storage to facilitate increased penetration of photovoltaic systems in electricity grids text January 2020
High-rate lithium ion energy storage to facilitate increased penetration of photovoltaic systems in electricity grids text January 2019

Figures / Tables (10)

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25 ENERGY STORAGE
freeze-casting
lithium-ion
tortuosity