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journal article·2024-05Open access

Competing Mechanisms Determine Oxygen Redox in Doped Ni–Mn Based Layered Oxides for Na‐Ion Batteries

Yongchun Li, Katherine A. Mazzio, Najma Yaqoob, Yanan Sun, Annica I. Freytag, Deniz Wong, Christian Schulz, Volodymyr Baran, Alba San Jose Mendez, Götz Schuck, Marcin Zając, Payam Kaghazchi, Philipp Adelhelm

Advanced Materials· Volume 36· Issue 18
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Source abstract

Abstract

Abstract Cation doping is an effective strategy for improving the cyclability of layered oxide cathode materials through suppression of phase transitions in the high voltage region. In this study, Mg and Sc are chosen as dopants in P2‐Na 0.67 Ni 0.33 Mn 0.67 O 2 , and both have found to positively impact the cycling stability, but influence the high voltage regime in different ways. Through a combination of synchrotron‐based methods and theoretical calculations it is shown that it is more than just suppression of the P2 to O2 phase transition that is critical for promoting the favorable properties, and that the interplay between Ni and O activity is also a critical aspect that dictates the performance. With Mg doping, the Ni activity can be enhanced while simultaneously suppressing the O activity. This is surprising because it is in contrast to what has been reported in other Mn‐based layered oxides where Mg is known to trigger oxygen redox. This contradiction is addressed by proposing a competing mechanism between Ni and Mg that impacts differences in O activity in Na 0.67 Mg x Ni 0.33‐ x Mn 0.67 O 2 ( x < 0 < 0.33). These findings provide a new direction in understanding the effects of cation doping on the electrochemical behavior of layered oxides.
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Research context

Energy storage

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

Institut für Chemie Humboldt‐University Berlin Brook‐Taylor‐Str. 2 12489 Berlin Germany

Joint Research Group "Operando Battery Analysis" (CE‐GOBA) Helmholtz‐Zentrum Berlin für Materialien und Energie, GmbH Hahn‐Meitner‐Platz 1 14109 Berlin Germany

Forschungszentrum Jülich GmbH Institute of Energy and Climate Research Materials Synthesis and Processing (IEK‐1) 52425 Jülich Germany

MESA+ Institute for Nanotechnology University of Twente Enschede 7500 AE The Netherlands

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

Deutsches Elektronen‐Synchrotron (DESY) Notkestraße 85 22607 Hamburg Germany

Department Structure and Dynamics of Energy Materials Helmholtz‐Zentrum Berlin für Materialien und Energie, GmbH Hahn‐Meitner‐Platz 1 14109 Berlin Germany

National Synchrotron Radiation Centre SOLARIS Jagiellonian University, ul Czerwone Maki 98 Kraków 30‐392 Poland

Funding

Deutsche Forschungsgemeinschaft · Bundesministerium für Bildung und Forschung

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