journal article·2024-01

Toward a Nanoscale‐Defect‐Free Ni‐Rich Layered Oxide Cathode Through Regulated Pore Evolution for Long‐Lifespan Li Rechargeable Batteries

Seok Hyun Song, Hwa Soo Kim, Kyoung Sun Kim, Seokjae Hong, Hyungkwon Jeon, Jun Lim, Young Hwa Jung, Hyungju Ahn, Jong Dae Jang, Man‐Ho Kim, Jong Hyeok Seo, Ji‐Hwan Kwon, Dokyung Kim, Young Joo Lee, Young‐Soo Han, Kyu‐Young Park, Chunjoong Kim, Seung‐Ho Yu, Hyeokjun Park, Hyeong Min Jin, Hyungsub Kim

Advanced Functional Materials· Volume 34· Issue 3
Publisher page

Abstract

Abstract Ni‐rich layered oxides are envisioned as the most promising cathode materials for next‐generation lithium‐ion batteries; however, their practical adoption is plagued by fast capacity decay originating from chemo‐mechanical degradation. The intrinsic chemical–mechanical instability, inherited from atomic‐ and nanoscale defects generated during synthesis, is not yet resolved. Here, atomic‐ and nanoscale structural evolution during solid‐state synthesis of Ni‐rich layered cathode, Li[Ni0.92Co0.03Mn0.05]O2, is investigated using combined X‐ray/neutron scattering and electron/X‐ray microscopy. The multiscale analyses demonstrate the intertwined correlation between phase transition and microstructural evolution, with atomic‐scale defects derived from the decomposition of precursors leading to the creation of intra/inter‐granular pores. The nucleation and coalescence mechanism of pore defects during the synthesis of Ni‐rich layered cathodes are quantitatively revealed. Furthermore, a modified synthetic route is proposed to effectively circumvent the formation of nanoscale defects in Ni‐rich layered cathodes by facilitating uniform synthetic reactions, resulting in superior electrochemical and microstructural stability.
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Research context

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

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

Affiliations

Neutron Science Division Korea Atomic Energy Research Institute (KAERI) 34057 111 Daedeok‐daero 989 Beon‐Gil, Yuseong‐gu Daejeon Republic of Korea

Department of Chemical and Biological Engineering Korea University 02841 145 Anam‐Ro, Seongbuk‐Gu Seoul Republic of Korea

Department of Organic Materials Engineering Chungnam National University 34134 Daejeon Republic of Korea

Department of Materials Science and Engineering Chungnam National University 34134 Daejeon Republic of Korea

Beamline Department Pohang Accelerator Laboratory 37673 Pohang Republic of Korea

Advanced Analysis Center Korea Institute of Science and Technology (KIST) 136–791 Seoul Republic of Korea

Interdisciplinary Materials Measurement Institute Korea Research Institute of Standards and Science (KRISS) 34113 Gajeongro 267, Yuseong‐gu Daejeon Republic of Korea

Western Seoul Center Korea Basic Science Institute (KBSI) 03759 150 Bugahyeon‐ro, Seodaemun‐gu Seoul Republic of Korea

Department of Chemistry Chung‐Ang University Seoul 06974 Republic of Korea

Department of Materials Science and Engineering Pohang University of Science and Technology (POSTECH) 37667 40, Jigok‐ro 212beon‐gil, Nam‐gu, Pohang‐si Gyeongsangbuk‐do Republic of Korea

Graduate Institute of Ferrous & Eco Materials Technology Pohang University of Science and Technology (POSTECH) 40, Jigok‐ro 212beon‐gil, Nam‐gu Pohang‐si Gyeongsangbuk‐do 37667 Republic of Korea

Funding

Korea Institute of Energy Technology Evaluation and Planning · Ministry of Science and ICT, South Korea

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