Mn versus Al in Layered Oxide Cathodes in Lithium-Ion Batteries: A Comprehensive Evaluation on Long-Term Cyclability

Li, Wangda; Liu, Xiaoming; Celio, Hugo; Smith, Patrick; Dolocan, Andrei; Chi, Miaofang; Manthiram, Arumugam

doi:10.1002/aenm.201703154

Title: Mn versus Al in Layered Oxide Cathodes in Lithium-Ion Batteries: A Comprehensive Evaluation on Long-Term Cyclability

Journal Article · Fri Feb 02 00:00:00 EST 2018 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.201703154· OSTI ID:1470844

Li, Wangda ^[1]; Liu, Xiaoming ^[2]; Celio, Hugo ^[1]; Smith, Patrick ^[1]; Dolocan, Andrei ^[1]; Chi, Miaofang ^[2];

^[1]

Univ. of Texas, Austin, TX (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

AbstractNickel‐rich layered oxide cathodes with the composition LiNi1−x−yCoxMnyO2 (NCM, (1−x−y) ≥ 0.6) are under intense scrutiny recently to contend with commercial LiNi0.8Co0.15Al0.05O2 (NCA) for high‐energy‐density batteries for electric vehicles. However, a comprehensive assessment of their electrochemical durability is currently lacking. Herein, two in‐house cathodes, LiNi0.8Co0.15Al0.05O2 and LiNi0.7Co0.15Mn0.15O2, are investigated in a high‐voltage graphite full cell over 1500 charge‐discharge cycles (≈5–10 year service life in vehicles). Despite a lower nickel content, NCM shows more performance deterioration than NCA. Critical underlying degradation processes, including chemical, structural, and mechanical aspects, are analyzed via an arsenal of characterization techniques. Overall, Mn substitution appears far less effective than Al in suppressing active mass dissolution and irreversible phase transitions of the layered oxide cathodes. The active mass dissolution (and crossover) accelerates capacity decline with sustained parasitic reactions on the graphite anode, while the phase transitions are primarily responsible for cell resistance increase and voltage fade. With Al doping, on the other hand, secondary particle pulverization is the more limiting factor for long‐term cyclability compared to Mn. These results establish a fundamental guideline for designing high‐performing Ni‐rich NCM cathodes as a compelling alternative to NCA and other compositions for electric vehicle applications.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of Texas, Austin, TX (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; DE‐EE0007762; EE0007762

OSTI ID:: 1470844

Alternate ID(s):: OSTI ID: 1419355; OSTI ID: 2217318

Journal Information:: Advanced Energy Materials, Vol. 8, Issue 15; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 187 works

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aluminum and manganese substitution
electron microscopy
lithium-ion batteries
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batteries
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Title: Mn versus Al in Layered Oxide Cathodes in Lithium-Ion Batteries: A Comprehensive Evaluation on Long-Term Cyclability

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