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Title: Synthetic Control of Kinetic Reaction Pathway and Cationic Ordering in High-Ni Layered Oxide Cathodes

Journal Article · · Advanced Materials
 [1];  [2];  [2];  [2];  [3];  [4];  [2];  [5];  [6];  [7];  [8];  [9];  [2];  [10];  [2]; ORCiD logo [3]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States); Xiamen Univ. (China)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States); Peking Univ. Shenzhen Graduate School (China)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  6. Cornell Univ., Ithaca, NY (United States)
  7. Peking Univ. Shenzhen Graduate School (China)
  8. Hayang Univ., Seoul (Korea, Republic of)
  9. Xiamen Univ. (China)
  10. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
+ Show Author Affiliations

Nickel-rich layered transition metal oxides, LiNi1-x(MnCo)(x)O-2 (1-x >= 0.5), are appealing candidates for cathodes in next-generation lithium-ion batteries (LIBs) for electric vehicles and other large-scale applications, due to their high capacity and low cost. However, synthetic control of the structural ordering in such a complex quaternary system has been a great challenge, especially in the presence of high Ni content. Herein, synthesis reactions for preparing layered LiNi0.7Mn0.15Co0.15O2 (NMC71515) by solid-state methods are investigated through a combination of time-resolved in situ high-energy X-ray diffraction and absorption spectroscopy measurements. The real-time observation reveals a strong temperature dependence of the kinetics of cationic ordering in NMC71515 as a result of thermal-driven oxidation of transition metals and lithium/oxygen loss that concomitantly occur during heat treatment. Through synthetic control of the kinetic reaction pathway, a layered NMC71515 with low cationic disordering and a high reversible capacity is prepared in air. The findings may help to pave the way for designing high-Ni layered oxide cathodes for LIBs.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE
Grant/Contract Number:
SC0012704; DE‐SC0012704; DE‐AC02‐06CH11357; AC05-00OR22725; AC02-06CH11357
OSTI ID:
1389227
Alternate ID(s):
OSTI ID: 1376967; OSTI ID: 1414679; OSTI ID: 1422578
Report Number(s):
BNL-114143-2017-JA
Journal Information:
Advanced Materials, Vol. 29, Issue 39; ISSN 0935-9648
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 100 works
Citation information provided by
Web of Science

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Cited By (12)

Challenges in Developing Electrodes, Electrolytes, and Diagnostics Tools to Understand and Advance Sodium-Ion Batteries journal February 2018
Ameliorating the Interfacial Problems of Cathode and Solid‐State Electrolytes by Interface Modification of Functional Polymers journal July 2018
Microstructure Evolution of Concentration Gradient Li[Ni 0.75 Co 0.10 Mn 0.15 ]O 2 Cathode for Lithium-Ion Batteries journal May 2018
Trace doping of multiple elements enables stable battery cycling of LiCoO2 at 4.6 V journal June 2019
Influence of Calcination Temperature on Structure and Electrochemical Behavior of LiNi0.83 Co0.11Mn0.06O2 Cathodes for Lithium-Ion Batteries journal January 2019
Use of Ce to Reinforce the Interface of Ni-Rich LiNi 0.8 Co 0.1 Mn 0.1 O 2 Cathode Materials for Lithium-Ion Batteries under High Operating Voltage journal January 2019
Identifying the Origin and Contribution of Surface Storage in TiO 2 (B) Nanotube Electrode by In Situ Dynamic Valence State Monitoring journal July 2018
Self-assembly of polyoxometalate/reduced graphene oxide composites induced by ionic liquids as a high-rate cathode for batteries: “killing two birds with one stone” journal January 2018
Investigating the Effects of Magnesium Doping in Various Ni-Rich Positive Electrode Materials for Lithium Ion Batteries journal January 2019
Surface/Interface Structure Degradation of Ni‐Rich Layered Oxide Cathodes toward Lithium‐Ion Batteries: Fundamental Mechanisms and Remedying Strategies journal December 2019
Increase and discretization of the energy barrier for individual LiNi x Co y Mn y O 2 ( x + 2 y =1) particles with the growth of a Li 2 CO 3 surface film journal January 2019
ZnNi x Mn x Co 2-2 x O 4 Spinel as a High-Voltage and High-Capacity Cathode Material for Nonaqueous Zn-Ion Batteries journal May 2018

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25 ENERGY STORAGE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY