Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Toward Long-Life, Ultrahigh-Nickel Layered Oxide Cathodes for Lithium-Ion Batteries: Optimizing the Interphase Chemistry with a Dual-Functional Polymer

Journal Article · · Chemistry of Materials
 [1];  [2];  [2]
  1. Univ. of Texas, Austin, TX (United States); University of Texas at Austin
  2. Univ. of Texas, Austin, TX (United States)
Boosting the Ni content in LiMO2 (M = Ni, Co, Mn, etc.) layered oxides is a promising way to establish high-energydensity, low-cost cathodes, but the poor cathode surface stability is a daunting challenge for their practical viability. Herein, by constructing a dual-functional binder framework with a conductive polymer - polyaniline (PANI), the ultrahigh-Ni layered oxide cathode (LiNi0.94Co0.06O2) exhibits significantly improved cyclability, with a capacity retention greatly increased from 47% to 81% over 1,000 cycles in full cells. It is demonstrated that the acidic species (e.g. HF) in the electrolyte can be efficiently scavenged through a protonation process of PANI, hence the cathode surface reactivity is greatly suppressed and the rock-salt phase propagation into bulk structure is considerably alleviated. Furthermore, the PANI binder system effectively prevents both the cathode-electrolyte interphase (CEI) and anode-electrolyte interphase (AEI) from degrading to a thick “triple-layer” architecture upon extensive cycling, resulting in more robust, thinner CEI and AEI with regulated interphasial chemistry. Moreover, the delocalized π-conjugated electrons along the backbone of PANI facilitate fast electron transfer and promote rate capability even at low temperatures (-20 °C). Finally, this work sheds light on rational binder engineering for developing high-energy-density lithium-ion batteries with acceptable cycle life.
Research Organization:
Univ. of Texas, Austin, TX (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); Welch Foundation
Grant/Contract Number:
EE0007762
OSTI ID:
2217334
Alternate ID(s):
OSTI ID: 1799357
Journal Information:
Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 2 Vol. 32; ISSN 0897-4756
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (38)

High-Performance Heterostructured Cathodes for Lithium-Ion Batteries with a Ni-Rich Layered Oxide Core and a Li-Rich Layered Oxide Shell journal May 2016
Understanding the Degradation Mechanisms of LiNi 0.5 Co 0.2 Mn 0.3 O 2 Cathode Material in Lithium Ion Batteries journal August 2013
A Novel Surface Treatment Method and New Insight into Discharge Voltage Deterioration for High-Performance 0.4Li 2 MnO 3- 0.6LiNi 1/3 Co 1/3 Mn 1/3 O 2 Cathode Materials journal June 2014
A Novel Electrolyte Salt Additive for Lithium-Ion Batteries with Voltages Greater than 4.7 V journal November 2016
Extending the Service Life of High-Ni Layered Oxides by Tuning the Electrode-Electrolyte Interphase journal September 2018
Ethylene Carbonate‐Free Electrolytes for High‐Nickel Layered Oxide Cathodes in Lithium‐Ion Batteries journal June 2019
There and Back Again-The Journey of LiNiO 2 as a Cathode Active Material journal May 2019
Adiponitrile-Lithium Bis(trimethylsulfonyl)imide Solutions as Alkyl Carbonate-free Electrolytes for Li 4 Ti 5 O 12 (LTO)/LiNi 1/3 Co 1/3 Mn 1/3 O 2 (NMC) Li-Ion Batteries journal April 2017
Nano‐Sized AlPO 4 Coating Layer on Graphite Powder to Improve the Electrochemical Properties of High‐Voltage Graphite/LiNi 0.5 Mn 1.5 O 4 Li‐Ion Cells journal June 2019
Electrochemical and physical characterization of lithium ionic salt doped polyaniline as a polymer electrode of lithium secondary battery journal April 2000
Binding energy referencing for XPS in alkali metal-based battery materials research (I): Basic model investigations journal October 2015
A Mild Surface Washing Method Using Protonated Polyaniline for Ni-rich LiNi 0.8 Co 0.1 Mn 0.1 O 2 Material of Lithium Ion Batteries journal September 2017
A perspective on nickel-rich layered oxide cathodes for lithium-ion batteries journal January 2017
Graphite and LiCo1/3Mn1/3Ni1/3O2 electrodes with piperidinium ionic liquid and lithium bis(fluorosulfonyl)imide for Li-ion batteries journal May 2012
Realizing superior cycling stability of Ni-Rich layered cathode by combination of grain boundary engineering and surface coating journal August 2019
Facilitating the Operation of Lithium-Ion Cells with High-Nickel Layered Oxide Cathodes with a Small Dose of Aluminum journal April 2018
Solid–Liquid Interfacial Reaction Trigged Propagation of Phase Transition from Surface into Bulk Lattice of Ni-Rich Layered Cathode journal September 2018
Toward Safe Lithium Metal Anode in Rechargeable Batteries: A Review journal July 2017
Electrode–Electrolyte Interface in Li-Ion Batteries: Current Understanding and New Insights journal October 2015
Long-Life Nickel-Rich Layered Oxide Cathodes with a Uniform Li 2 ZrO 3 Surface Coating for Lithium-Ion Batteries journal March 2017
An Outlook on Lithium Ion Battery Technology journal September 2017
Acid-Scavenging Separators: A Novel Route for Improving Li-Ion Batteries’ Durability journal September 2017
Revealing Cycling Rate-Dependent Structure Evolution in Ni-Rich Layered Cathode Materials journal September 2018
Challenges for Rechargeable Li Batteries journal February 2010
Electrolytes and Interphases in Li-Ion Batteries and Beyond journal October 2014
First Evidence of Manganese–Nickel Segregation and Densification upon Cycling in Li-Rich Layered Oxides for Lithium Batteries journal July 2013
Surface reconstruction and chemical evolution of stoichiometric layered cathode materials for lithium-ion batteries journal March 2014
Coupling of electrochemically triggered thermal and mechanical effects to aggravate failure in a layered cathode journal June 2018
Tailoring grain boundary structures and chemistry of Ni-rich layered cathodes for enhanced cycle stability of lithium-ion batteries journal June 2018
Stable cycling of high-voltage lithium metal batteries in ether electrolytes journal July 2018
Preparation and Properties of A Hyperbranch-Structured Polyamine adsorbent for Carbon Dioxide Capture journal June 2017
Role of fluorine surface modification in improving electrochemical cyclability of concentration gradient Li[Ni 0.73 Co 0.12 Mn 0.15 ]O 2 cathode material for Li-ion batteries journal January 2016
A review of Ni-based layered oxides for rechargeable Li-ion batteries journal January 2017
Polyanilines: a novel class of conducting polymers journal January 1989
Improved Conducting States Induced by an Electrochemical Charging Process in Polyaniline Film Doped with New Dopants journal January 2002
Enhanced Electrochemical Properties of LiNi 0.8 Co 0.1 Mn 0.1 O 2 at Elevated Temperature by Simultaneous Structure and Interface Regulating journal January 2019
Improving the Performance of Graphite/ LiNi 0.5 Mn 1.5 O 4 Cells at High Voltage and Elevated Temperature with Added Lithium Bis(oxalato) Borate (LiBOB) journal January 2013
Binding Energy Referencing for XPS in Alkali Metal-Based Battery Materials Research (II): Application to Complex Composite Electrodes journal August 2018

Similar Records

A Comprehensive Analysis of the Interphasial and Structural Evolution over Long–Term Cycling of Ultrahigh–Nickel Cathodes in Lithium–Ion Batteries
Journal Article · Sun Oct 27 20:00:00 EDT 2019 · Advanced Energy Materials · OSTI ID:2217333

Extending the Service Life of High–Ni Layered Oxides by Tuning the Electrode–Electrolyte Interphase
Journal Article · Sun Sep 09 20:00:00 EDT 2018 · Advanced Energy Materials · OSTI ID:2217319