journal article·2025-11-04

Unlocking the Potential of Cobalt-Free Lithium-Ion Cathodes via Lithium-Rich Disorder Domains

Hao Liu, Hang Li, Weibo Hua, Bixian Ying, Karin Kleiner, Jing Lin, Hang Xu, Bijian Deng, Deniz Wong, Thomas Bergfeldt, Stefan Mangold, Peter Nagel, Stefan Schuppler, Michael Merz, Volodymyr Baran, Wei Xiang, Yongjian Li, Ning Li, Michael Knapp, Helmut Ehrenberg, Sylvio Indris

ACS Nano· Volume 19· Issue 43
Publisher page

Abstract

High-voltage, low-nickel, cobalt-free layered oxides are promising candidates for high-energy-density lithium-ion batteries. However, their practical application is hindered by intrinsic cation disorder and structural degradation at high voltages, leading to a poor electrochemical performance. Here, we report a slightly lithium-enriched, cobalt-free layered oxide, Li 1.05 Ni 0.43 Mn 0.52 O 2, featuring lithium-rich disorder domains achieved through chemical composition optimization. Advanced structural characterization demonstrates that nickel ions not only reside within the TM layers but also occupy the Li layers, acting as pinned ions. Theoretical calculations indicate that this in-plane and out-of-plane disorder enables reversible oxygen redox activity without oxygen release at high voltages. Moreover, this local structural framework preserves integrity even after extended cycling, ensuring chemical and structural stability during battery operation. Consequently, the cathode delivers an impressive discharge capacity of 202.2 mAh g –1 at C/10 and exceptional cycling stability, retaining 96.3% of its capacity after 200 cycles at C/3 within a voltage range of 2.5–4.55 V. Our findings provide valuable insights into the design of high-energy-density, cobalt-free layered cathodes.
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Research context

OpenAlex topics: Advancements in Battery Materials · Advanced Battery Technologies Research · Advanced Battery Materials and Technologies

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

Affiliations

Institute for Applied Materials (IAM), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1, Eggenstein-Leopoldshafen 76344, Germany

School of Advanced Materials

Peking University, Shenzhen Graduate School

School of Chemical Engineering and Technology, Xi’an Jiaotong University, No.28, West Xianning Road, Xi’an, Shaanxi 710049, China

Münster Electrochemical Energy Technology (MEET)

University of Münster (WWU)

Institute of Nanotechnology (INT), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1, Eggenstein-Leopoldshafen 76344, Germany

Department of Materials, University of Oxford, Parks Road, Oxford OX1 3PH, U.K.

Dynamics and Transport in Quantum Materials, Helmholtz-Zentrum Berlin für Materialen und Energie, GmbH, Albert-Einstein-Strasse 15, Berlin 12489, Germany

Institute for Photon Science and Synchrotron Radiation (IPS), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1, Eggenstein-Leopoldshafen 76344, Germany

Karlsruhe Nano Micro Facility, Karlsruhe Institute of Technology (KIT), Kaiserstraße 12, Karlsruhe 76131, Germany

Institute for Quantum Materials and Technologies, Karlsruhe Institute of Technology (KIT), Kaiserstraße 12, Karlsruhe 76131, Germany

Deutsches Elektronen-Synchrotron (DESY), Notkestrasse 85, Hamburg 22607, Germany

College of Materials and Chemistry & Chemical Engineering (College of Lithium Resources and Lithium Battery Industry)

Chengdu University of Technology

School of Materials Science and Engineering, Beijing Key Laboratory of Environmental Science and Engineering

Beijing Institute of Technology

Applied Chemistry and Engineering Research Centre of Excellence (ACER CoE), Université Mohammed VI Polytechnique (UM6P), Lot 660, Hay Moulay Rachid, Ben Guerir 43150, Morocco

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