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journal article·2022-01Open access

Elucidating and Mitigating High‐Voltage Degradation Cascades in Cobalt‐Free LiNiO2 Lithium‐Ion Battery Cathodes

Kyu‐Young Park, Yizhou Zhu, Carlos G. Torres‐Castanedo, Hee Joon Jung, Norman S. Luu, Ozge Kahvecioglu, Yiseul Yoo, Jung‐Woo T. Seo, Julia R. Downing, Hee‐Dae Lim, Michael J. Bedzyk, Christopher Wolverton, Mark C. Hersam

Advanced Materials· Volume 34· Issue 3
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Abstract

Abstract LiNiO2 (LNO) is a promising cathode material for next‐generation Li‐ion batteries due to its exceptionally high capacity and cobalt‐free composition that enables more sustainable and ethical large‐scale manufacturing. However, its poor cycle life at high operating voltages over 4.1 V impedes its practical use, thus motivating efforts to elucidate and mitigate LiNiO2 degradation mechanisms at high states of charge. Here, a multiscale exploration of high‐voltage degradation cascades associated with oxygen stacking chemistry in cobalt‐free LiNiO2, is presented. Lattice oxygen loss is found to play a critical role in the local O3–O1 stacking transition at high states of charge, which subsequently leads to Ni‐ion migration and irreversible stacking faults during cycling. This undesirable atomic‐scale structural evolution accelerates microscale electrochemical creep, cracking, and even bending of layers, ultimately resulting in macroscopic mechanical degradation of LNO particles. By employing a graphene‐based hermetic surface coating, oxygen loss is attenuated in LNO at high states of charge, which suppresses the initiation of the degradation cascade and thus substantially improves the high‐voltage capacity retention of LNO. Overall, this study provides mechanistic insight into the high‐voltage degradation of LNO, which will inform ongoing efforts to employ cobalt‐free cathodes in Li‐ion battery technology.
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Research context

Energy storageNanomaterials

OpenAlex topics: Advancements in Battery Materials · Supercapacitor Materials and Fabrication · Advanced Battery Materials and Technologies

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Materials Science and Engineering Northwestern University Evanston IL 60208 USA

Graduate Institute of Ferrous and Energy Materials Technology Pohang University of Science and Technology Pohang Kyungbuk 37673 Republic of Korea

NUANCE Center Northwestern University 2220 Campus Drive Evanston IL 60208 USA

Argonne National Laboratory Applied Materials Division 9700 South Cass Avenue Lemont IL 60439 USA

Center for Energy Storage Research Korea Institute of Science and Technology (KIST) Hwarang‐ro 14‐gil 5, Seongbuk‐gu Seoul 02792 Republic of Korea

Department of Materials Science and Engineering Korea University 145, Anam‐ro, Seongbuk‐gu Seoul 02841 Republic of Korea

Volexion, Inc. 4809 North Ravenswood Avenue Chicago IL 60640 USA

Department of Physics and Astronomy Northwestern University Evanston IL 60208 USA

Department of Chemistry Northwestern University Evanston IL 60208 USA

Department of Electrical and Computer Engineering Northwestern University Evanston IL 60208 USA

Funding

U.S. Department of Energy · Office of Science · Basic Energy Sciences · National Research Foundation of Korea · Ministry of Education · Materials Research Science and Engineering Center, Harvard University · Argonne National Laboratory

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