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Title: Insights into Li/Ni ordering and surface reconstruction during synthesis of Ni-rich layered oxides

Abstract

Nickel-rich layered transition metal oxides (NMCs) have been intensively studied as promising cathode candidates for next-generation Li-ion batteries, known for low cost and high theoretical capacity. However, the practical capacity of NMCs is largely determined by cationic ordering and has yet to be well controlled during synthesis, largely due to the complexity and non-equilibrium nature of the reactions occurring in the sintering process. In this work, high-energy synchrotron X-ray diffraction is employed to investigate the kinetic and thermodynamic aspects of cationic ordering during synthesis of LiNi0.7Mn0.15Co0.15O2 (NMC71515). It is found that cationic ordering in the bulk is coupled to surface reconstruction during synthesis, occurring concomitantly and both being greatly affected by Li2CO3 decomposition and Li loss at the particle surface. Through tuning the sintering temperature and time, highly ordered NMC71515 with high capacity and excellent rate capability is synthesized. The developed approach may be applied broadly to the synthesis of high-performance Ni-rich NMC and other cathode materials.

Authors:
 [1]; ORCiD logo [2];  [1];  [3];  [4]; ORCiD logo [3]; ORCiD logo [2];  [5]
  1. Peking Univ., Shenzhen (China). Shenzhen Graduate School, School of Advanced Materials; Brookhaven National Lab. (BNL), Upton, NY (United States). Sustainable Energy Technologies Dept.
  2. Peking Univ., Shenzhen (China). Shenzhen Graduate School, School of Advanced Materials
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Electrochemical Technology Program, Chemical Sciences and Engineering Division
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States). Sustainable Energy Technologies Dept.
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC); Shenzhen Science and Technology
OSTI Identifier:
1492790
Alternate Identifier(s):
OSTI ID: 1485336
Report Number(s):
BNL-210927-2019-JAAM
Journal ID: ISSN 2050-7488; JMCAET
Grant/Contract Number:  
SC0012704; JCYJ20150729111733470; JCYJ20151015162256516
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 7; Journal Issue: 2; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 36 MATERIALS SCIENCE

Citation Formats

Duan, Yandong, Yang, Luyi, Zhang, Ming-Jian, Chen, Zonghai, Bai, Jianming, Amine, Khalil, Pan, Feng, and Wang, Feng. Insights into Li/Ni ordering and surface reconstruction during synthesis of Ni-rich layered oxides. United States: N. p., 2018. Web. doi:10.1039/C8TA10553G.
Duan, Yandong, Yang, Luyi, Zhang, Ming-Jian, Chen, Zonghai, Bai, Jianming, Amine, Khalil, Pan, Feng, & Wang, Feng. Insights into Li/Ni ordering and surface reconstruction during synthesis of Ni-rich layered oxides. United States. doi:10.1039/C8TA10553G.
Duan, Yandong, Yang, Luyi, Zhang, Ming-Jian, Chen, Zonghai, Bai, Jianming, Amine, Khalil, Pan, Feng, and Wang, Feng. Tue . "Insights into Li/Ni ordering and surface reconstruction during synthesis of Ni-rich layered oxides". United States. doi:10.1039/C8TA10553G. https://www.osti.gov/servlets/purl/1492790.
@article{osti_1492790,
title = {Insights into Li/Ni ordering and surface reconstruction during synthesis of Ni-rich layered oxides},
author = {Duan, Yandong and Yang, Luyi and Zhang, Ming-Jian and Chen, Zonghai and Bai, Jianming and Amine, Khalil and Pan, Feng and Wang, Feng},
abstractNote = {Nickel-rich layered transition metal oxides (NMCs) have been intensively studied as promising cathode candidates for next-generation Li-ion batteries, known for low cost and high theoretical capacity. However, the practical capacity of NMCs is largely determined by cationic ordering and has yet to be well controlled during synthesis, largely due to the complexity and non-equilibrium nature of the reactions occurring in the sintering process. In this work, high-energy synchrotron X-ray diffraction is employed to investigate the kinetic and thermodynamic aspects of cationic ordering during synthesis of LiNi0.7Mn0.15Co0.15O2 (NMC71515). It is found that cationic ordering in the bulk is coupled to surface reconstruction during synthesis, occurring concomitantly and both being greatly affected by Li2CO3 decomposition and Li loss at the particle surface. Through tuning the sintering temperature and time, highly ordered NMC71515 with high capacity and excellent rate capability is synthesized. The developed approach may be applied broadly to the synthesis of high-performance Ni-rich NMC and other cathode materials.},
doi = {10.1039/C8TA10553G},
journal = {Journal of Materials Chemistry. A},
number = 2,
volume = 7,
place = {United States},
year = {2018},
month = {12}
}

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