Revealing the inhomogeneous surface chemistry on the spherical layered oxide polycrystalline cathode particles

doi:10.1088/1674-1056/ab6585

中国物理B ›› 2020, Vol. 29 ›› Issue (2): 26103-026103.doi: 10.1088/1674-1056/ab6585

所属专题： SPECIAL TOPIC — Advanced calculation & characterization of energy storage materials & devices at multiple scale

• SPECIAL TOPIC—Recent advances in thermoelectric materials and devices • 上一篇下一篇

Revealing the inhomogeneous surface chemistry on the spherical layered oxide polycrystalline cathode particles

Zhi-Sen Jiang(蒋之森), Shao-Feng Li(李少锋), Zheng-Rui Xu(许正瑞), Dennis Nordlund, Hendrik Ohldag, Piero Pianetta, Jun-Sik Lee, Feng Lin(林锋), Yi-Jin Liu(刘宜晋)

1 College of Physics, Sichuan University, Chengdu 610065, China;
2 Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA;
3 Department of Chemistry, Virginia Tech, Blacksburg, VA 24061, USA

收稿日期:2019-11-16 修回日期:2019-12-20 出版日期:2020-02-05 发布日期:2020-02-05
通讯作者: Jun-Sik Lee, Feng Lin, Yi-Jin Liu E-mail:jslee@slac.stanford.edu;fenglin@vt.edu;liuyijin@slac.stanford.edu
基金资助:
Project supported by U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515 and National Science Foundation under Grant No. DMR-1832613.

Revealing the inhomogeneous surface chemistry on the spherical layered oxide polycrystalline cathode particles

Zhi-Sen Jiang(蒋之森)¹, Shao-Feng Li(李少锋)², Zheng-Rui Xu(许正瑞)³, Dennis Nordlund², Hendrik Ohldag², Piero Pianetta², Jun-Sik Lee², Feng Lin(林锋)³, Yi-Jin Liu(刘宜晋)²

1 College of Physics, Sichuan University, Chengdu 610065, China;
2 Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA;
3 Department of Chemistry, Virginia Tech, Blacksburg, VA 24061, USA

Received:2019-11-16 Revised:2019-12-20 Online:2020-02-05 Published:2020-02-05
Contact: Jun-Sik Lee, Feng Lin, Yi-Jin Liu E-mail:jslee@slac.stanford.edu;fenglin@vt.edu;liuyijin@slac.stanford.edu
Supported by:
Project supported by U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515 and National Science Foundation under Grant No. DMR-1832613.

摘要/Abstract

摘要： The hierarchical structure of the composite cathodes brings in significant chemical complexity related to the interfaces, such as cathode electrolyte interphase. These interfaces account for only a small fraction of the volume and mass, they could, however, have profound impacts on the cell-level electrochemistry. As the investigation of these interfaces becomes a crucial topic in the battery research, there is a need to properly study the surface chemistry, particularly to eliminate the biased, incomplete characterization provided by techniques that assume the homogeneous surface chemistry. Herein, we utilize nano-resolution spatially-resolved x-ray spectroscopic tools to probe the heterogeneity of the surface chemistry on LiNi_0.8Mn_0.1Co_0.1O₂ layered cathode secondary particles. Informed by the nano-resolution mapping of the Ni valance state, which serves as a measurement of the local surface chemistry, we construct a conceptual model to elucidate the electrochemical consequence of the inhomogeneous local impedance over the particle surface. Going beyond the implication in battery science, our work highlights a balance between the high-resolution probing the local chemistry and the statistical representativeness, which is particularly vital in the study of the highly complex material systems.

关键词: Ni-rich cathode, x-ray nanoprobe, redox heterogeneity, surface chemistry

Abstract: The hierarchical structure of the composite cathodes brings in significant chemical complexity related to the interfaces, such as cathode electrolyte interphase. These interfaces account for only a small fraction of the volume and mass, they could, however, have profound impacts on the cell-level electrochemistry. As the investigation of these interfaces becomes a crucial topic in the battery research, there is a need to properly study the surface chemistry, particularly to eliminate the biased, incomplete characterization provided by techniques that assume the homogeneous surface chemistry. Herein, we utilize nano-resolution spatially-resolved x-ray spectroscopic tools to probe the heterogeneity of the surface chemistry on LiNi_0.8Mn_0.1Co_0.1O₂ layered cathode secondary particles. Informed by the nano-resolution mapping of the Ni valance state, which serves as a measurement of the local surface chemistry, we construct a conceptual model to elucidate the electrochemical consequence of the inhomogeneous local impedance over the particle surface. Going beyond the implication in battery science, our work highlights a balance between the high-resolution probing the local chemistry and the statistical representativeness, which is particularly vital in the study of the highly complex material systems.

Key words: Ni-rich cathode, x-ray nanoprobe, redox heterogeneity, surface chemistry

中图分类号: (X-ray absorption spectroscopy: EXAFS, NEXAFS, XANES, etc.)

61.05.cj

78.70.Dm (X-ray absorption spectra) 87.59.-e (X-ray imaging) 82.45.Fk (Electrodes)

蒋之森, 李少锋, 许正瑞, Dennis Nordlund, Hendrik Ohldag, Piero Pianetta, Jun-Sik Lee, 林锋, 刘宜晋. Revealing the inhomogeneous surface chemistry on the spherical layered oxide polycrystalline cathode particles[J]. 中国物理B, 2020, 29(2): 26103-026103.

Zhi-Sen Jiang(蒋之森), Shao-Feng Li(李少锋), Zheng-Rui Xu(许正瑞), Dennis Nordlund, Hendrik Ohldag, Piero Pianetta, Jun-Sik Lee, Feng Lin(林锋), Yi-Jin Liu(刘宜晋). Revealing the inhomogeneous surface chemistry on the spherical layered oxide polycrystalline cathode particles[J]. Chin. Phys. B, 2020, 29(2): 26103-026103.

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Revealing the inhomogeneous surface chemistry on the spherical layered oxide polycrystalline cathode particles

Revealing the inhomogeneous surface chemistry on the spherical layered oxide polycrystalline cathode particles

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