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

Abstract

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.

Authors:
 [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)
Publication Date:
Research Org.:
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 Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE
OSTI Identifier:
1389227
Alternate Identifier(s):
OSTI ID: 1376967; OSTI ID: 1414679; OSTI ID: 1422578
Report Number(s):
BNL-114143-2017-JA
Journal ID: ISSN 0935-9648
Grant/Contract Number:  
SC0012704; DE‐SC0012704; DE‐AC02‐06CH11357; AC05-00OR22725; AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 29; Journal Issue: 39; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Wang, Dawei, Kou, Ronghui, Ren, Yang, Sun, Cheng-Jun, Zhao, Hu, Zhang, Ming-Jian, Li, Yan, Huq, Ashifia, Ko, J. Y. Peter, Pan, Feng, Sun, Yang-Kook, Yang, Yong, Amine, Khalil, Bai, Jianming, Chen, Zonghai, and Wang, Feng. Synthetic Control of Kinetic Reaction Pathway and Cationic Ordering in High-Ni Layered Oxide Cathodes. United States: N. p., 2017. Web. doi:10.1002/adma.201606715.
Wang, Dawei, Kou, Ronghui, Ren, Yang, Sun, Cheng-Jun, Zhao, Hu, Zhang, Ming-Jian, Li, Yan, Huq, Ashifia, Ko, J. Y. Peter, Pan, Feng, Sun, Yang-Kook, Yang, Yong, Amine, Khalil, Bai, Jianming, Chen, Zonghai, & Wang, Feng. Synthetic Control of Kinetic Reaction Pathway and Cationic Ordering in High-Ni Layered Oxide Cathodes. United States. https://doi.org/10.1002/adma.201606715
Wang, Dawei, Kou, Ronghui, Ren, Yang, Sun, Cheng-Jun, Zhao, Hu, Zhang, Ming-Jian, Li, Yan, Huq, Ashifia, Ko, J. Y. Peter, Pan, Feng, Sun, Yang-Kook, Yang, Yong, Amine, Khalil, Bai, Jianming, Chen, Zonghai, and Wang, Feng. 2017. "Synthetic Control of Kinetic Reaction Pathway and Cationic Ordering in High-Ni Layered Oxide Cathodes". United States. https://doi.org/10.1002/adma.201606715. https://www.osti.gov/servlets/purl/1389227.
@article{osti_1389227,
title = {Synthetic Control of Kinetic Reaction Pathway and Cationic Ordering in High-Ni Layered Oxide Cathodes},
author = {Wang, Dawei and Kou, Ronghui and Ren, Yang and Sun, Cheng-Jun and Zhao, Hu and Zhang, Ming-Jian and Li, Yan and Huq, Ashifia and Ko, J. Y. Peter and Pan, Feng and Sun, Yang-Kook and Yang, Yong and Amine, Khalil and Bai, Jianming and Chen, Zonghai and Wang, Feng},
abstractNote = {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.},
doi = {10.1002/adma.201606715},
url = {https://www.osti.gov/biblio/1389227}, journal = {Advanced Materials},
issn = {0935-9648},
number = 39,
volume = 29,
place = {United States},
year = {Fri Aug 25 00:00:00 EDT 2017},
month = {Fri Aug 25 00:00:00 EDT 2017}
}

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Works referencing / citing this record:

Challenges in Developing Electrodes, Electrolytes, and Diagnostics Tools to Understand and Advance Sodium-Ion Batteries
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Ameliorating the Interfacial Problems of Cathode and Solid‐State Electrolytes by Interface Modification of Functional Polymers
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Microstructure Evolution of Concentration Gradient Li[Ni 0.75 Co 0.10 Mn 0.15 ]O 2 Cathode for Lithium-Ion Batteries
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Trace doping of multiple elements enables stable battery cycling of LiCoO2 at 4.6 V
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Investigating the Effects of Magnesium Doping in Various Ni-Rich Positive Electrode Materials for Lithium Ion Batteries
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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
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