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In Situ Probing and Synthetic Control of Cationic Ordering in Ni-Rich Layered Oxide Cathodes

Journal Article · · Advanced Energy Materials
 [1];  [1];  [2];  [3];  [4];  [4];  [1];  [1];  [5];  [5];  [6];  [1];  [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Alfred Univ., NY (United States)
  4. Louisiana State Univ., Baton Rouge, LA (United States)
  5. Argonne National Lab. (ANL), Argonne, IL (United States)
  6. Peking Univ. Shenzhen Graduate School, Shenzhen (China)
+ Show Author Affiliations
Ni-rich layered oxides (LiNi1-xMxO2; M=Co, Mn, …) are appealing alternatives to conventional LiCoO2 as cathodes in Li-ion batteries for automobile and other large-scale applications due to their high theoretical capacity and low cost. However, preparing stoichiometric LiNi1-xMxO2 with ordered layer structure and high reversible capacity, has proven difficult due to Ni2+/Li+ cation mixing in octahedral sites. Herein, we report on in-situ studies of synthesis reactions and the associated structural ordering in preparing LiNiO2 and the Co-substituted variant, LiNi0.8Co0.2O2, thereby gaining insights into synthetic control of the structure and electrochemical properties of Ni-rich layered oxides. Results from this study indicate a direct transformation of the intermediate from the rock salt structure into hexagonal phase, and during the process, Co substitution facilities the nucleation of a Co-rich layered phase at low temperatures and subsequent growth and stabilization of solid solution Li(Ni, Co)O2 upon heat treatment in a highly oxidation environment. Optimal conditions were identified from the in-situ studies and utilized in obtaining stoichiometric LiNi0.8Co0.2O2 that exhibits high capacity of about 200 mAh/g with excellent retention. The findings shed light on designing Ni-rich layered oxide cathodes with enhanced electrochemical properties through synthetic control of the structural ordering in the materials.
Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0012704
OSTI ID:
1389223
Alternate ID(s):
OSTI ID: 1401242
OSTI ID: 1406900
OSTI ID: 1768777
Report Number(s):
BNL--114130-2017-JA; BNL--221104-2021-JAAM
Journal Information:
Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 3 Vol. 7; ISSN 1614-6832
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (14)

Surface/Interface Structure Degradation of Ni‐Rich Layered Oxide Cathodes toward Lithium‐Ion Batteries: Fundamental Mechanisms and Remedying Strategies journal December 2019
Challenges in Developing Electrodes, Electrolytes, and Diagnostics Tools to Understand and Advance Sodium-Ion Batteries journal February 2018
Radially Oriented Single‐Crystal Primary Nanosheets Enable Ultrahigh Rate and Cycling Properties of LiNi 0.8 Co 0.1 Mn 0.1 O 2 Cathode Material for Lithium‐Ion Batteries journal February 2019
Ti‐Gradient Doping to Stabilize Layered Surface Structure for High Performance High‐Ni Oxide Cathode of Li‐Ion Battery journal September 2019
Cooling Induced Surface Reconstruction during Synthesis of High‐Ni Layered Oxides journal October 2019
A Generalizable Top-Down Nanostructuring Method of Bulk Oxides: Sequential Oxygen-Nitrogen Exchange Reaction journal May 2018
High-voltage performance of concentration-gradient Li[Ni 0.6 Co 0.2 Mn 0.2 ]O 2 layered oxide cathode materials for lithium batteries journal January 2018
Theoretical investigation of the cation antisite defect in layer-structured cathode materials for Li-ion batteries journal January 2019
Thermally-driven mesopore formation and oxygen release in delithiated NCA cathode particles journal January 2019
Structure- and porosity-tunable, thermally reactive metal organic frameworks for high-performance Ni-rich layered oxide cathode materials with multi-scale pores journal January 2019
Enhanced high-voltage cycling stability of Ni-rich cathode materials via the self-assembly of Mn-rich shells journal January 2019
Laser processed Ni-Fe alloys as electrocatalyst toward oxygen evolution reaction journal June 2018
Probing the Nature of Li + /Ni 2+ Disorder on the Structure and Electrochemical Performance in Ni-Based Layered Oxide Cathodes journal January 2019
Ultrathin Al2O3 Coating on LiNi0.8Co0.1Mn0.1O2 Cathode Material for Enhanced Cycleability at Extended Voltage Ranges journal February 2019

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