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Accelerated Development of High Voltage Li‐Ion Cathodes

Accelerated Development of High Voltage Li‐Ion Cathodes High voltage cathodes are attractive for high energy density Li‐ion batteries. However, candidates such as LiCoPO4 have presented numerous challenges stemming from poor electronic/ionic conductivities such that typical solutions involving nanosizing result in extremely poor cycling performance. Here, high‐throughput methods are applied to develop near‐micron sized carbon‐coated LiCoPO4 with improved energy density and capacity retention. In total, 1300 materials with 46 different substituents are synthesized and characterized. A number of substituents show greatly improved capacity (e.g., 160 mAh g−1 for 1% indium (In) substitution vs 95 mAh g−1 for the pristine). However, co‐doping is required to improve extended cycling. Li1–3xCo1–2xInxMoxPO4 is found to be particularly effective with dramatically improved cycling (as high as 100% after 10 cycles, vs ≈50% in unsubstituted). While In improves the electronic conductivity of the carbon‐coated materials, molybdenum (Mo) co‐doping gives larger particles. DFT calculations show that Mo impedes the formation of Li/Co antisite defects. http://www.deepdyve.com/assets/images/DeepDyve-Logo-lg.png Advanced Energy Materials Wiley

Accelerated Development of High Voltage Li‐Ion Cathodes

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Publisher
Wiley
Copyright
© 2022 Wiley‐VCH GmbH
ISSN
1614-6832
eISSN
1614-6840
DOI
10.1002/aenm.202201704
Publisher site
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Abstract

High voltage cathodes are attractive for high energy density Li‐ion batteries. However, candidates such as LiCoPO4 have presented numerous challenges stemming from poor electronic/ionic conductivities such that typical solutions involving nanosizing result in extremely poor cycling performance. Here, high‐throughput methods are applied to develop near‐micron sized carbon‐coated LiCoPO4 with improved energy density and capacity retention. In total, 1300 materials with 46 different substituents are synthesized and characterized. A number of substituents show greatly improved capacity (e.g., 160 mAh g−1 for 1% indium (In) substitution vs 95 mAh g−1 for the pristine). However, co‐doping is required to improve extended cycling. Li1–3xCo1–2xInxMoxPO4 is found to be particularly effective with dramatically improved cycling (as high as 100% after 10 cycles, vs ≈50% in unsubstituted). While In improves the electronic conductivity of the carbon‐coated materials, molybdenum (Mo) co‐doping gives larger particles. DFT calculations show that Mo impedes the formation of Li/Co antisite defects.

Journal

Advanced Energy Materials – Wiley

Published: Oct 1, 2022

Keywords: combinatorial synthesis and electrochemistry; density functional theory calculations; high voltage cathodes for Li‐ion batteries; high‐throughput screening; X‐ray diffraction

References