Concerted Effect of Ion- and Electron-Conductive Additives on the Electrochemical and Thermal Performances of the LiNi0.8Co0.1Mn0.1O2 Cathode Material Synthesized by a Taylor-Flow Reactor for Lithium-Ion Batteries

Tadesu Hailu Mengesha; Juliya Jeyakumar; Yola Bertilsya Hendri; Yi-Shiuan Wu; Chun-Chen Yang; Quoc-Thai Pham; Chorng-Shyan Chern; Gunther Brunklaus; Martin Winter; Bing Joe Hwang

doi:10.1021/acsami.3c19386

Concerted Effect of Ion- and Electron-Conductive Additives on the Electrochemical and Thermal Performances of the LiNi_0.8Co_0.1Mn_0.1O₂ Cathode Material Synthesized by a Taylor-Flow Reactor for Lithium-Ion Batteries

ACS Appl Mater Interfaces. 2024 Apr 12. doi: 10.1021/acsami.3c19386. Online ahead of print.

Authors

Tadesu Hailu Mengesha^{1

2}, Juliya Jeyakumar¹, Yola Bertilsya Hendri¹, Yi-Shiuan Wu¹, Chun-Chen Yang^{1

3

4}, Quoc-Thai Pham⁵, Chorng-Shyan Chern⁶, Gunther Brunklaus⁷, Martin Winter^{7

8}, Bing Joe Hwang⁶

Affiliations

¹ Battery Research Center of Green Energy, Ming Chi University of Technology, New Taipei City 243303, Taiwan, ROC.
² College of Natural and Computational Science, Department of Chemistry, Wolkite University, Wolkite 07, SNNPR, Ethiopia.
³ Department of Chemical Engineering, Ming Chi University of Technology, New Taipei City 243303, Taiwan, ROC.
⁴ Department of Chemical and Materials Engineering & Center for Sustainability and Energy Technologies, Chang Gung University, Taoyuan City 333323, Taiwan.
⁵ Department of Chemical and Materials Engineering, National Ilan University, Yilan County, Yilan City, 260007, Taiwan, ROC.
⁶ Department of Chemical Engineering, National Taiwan University of Science and Technology, Taipei City 106335, Taiwan, ROC.
⁷ Helmholtz Institute Münster, IEK-12, Forschungszentrum Jülich GmbH, Corrensstraße 46, Münster 48149, Germany.
⁸ University of Münster, MEET Battery Research Center, Institute of Physical Chemistry, Corrensstraße 46, Münster 48149, Germany.

PMID: 38606845
DOI: 10.1021/acsami.3c19386

Abstract

To address the issue that a single coating agent cannot simultaneously enhance Li⁺-ion transport and electronic conductivity of Ni-rich cathode materials with surface modification, in the present study, we first successfully synthesized a LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811) cathode material by a Taylor-flow reactor followed by surface coating with Li-BTJ and dispersion of vapor-grown carbon fibers treated with polydopamine (PDA-VGCF) filler in the composite slurry. The Li-BTJ hybrid oligomer coating can suppress side reactions and enhance ionic conductivity, and the PDA-VGCFs filler can increase electronic conductivity. As a result of the synergistic effect of the dual conducting agents, the cells based on the modified NCM811 electrodes deliver superior cycling stability and rate capability, as compared to the bare NCM811 electrode. The CR2032 coin-type cells with the NCM811@Li-BTJ + PDA-VGCF electrode retain a discharge specific capacity of ∼92.2% at 1C after 200 cycles between 2.8 and 4.3 V (vs Li/Li⁺), while bare NCM811 retains only 84.0%. Moreover, the NCM811@Li-BTJ + PDA-VGCF electrode-based cells reduced the total heat (Q_t) by ca. 7.0% at 35 °C over the bare electrode. Remarkably, the Li-BTJ hybrid oligomer coating on the surface of the NCM811 active particles acts as an artificial cathode electrolyte interphase (ACEI) layer, mitigating irreversible surface phase transformation of the layered NCM811 cathode and facilitating Li⁺ ion transport. Meanwhile, the fiber-shaped PDA-VGCF filler significantly reduced microcrack propagation during cycling and promoted the electronic conductance of the NCM811-based electrode. Generally, enlightened with the current experimental findings, the concerted ion and electron conductive agents significantly enhanced the Ni-rich cathode-based cell performance, which is a promising strategy to apply to other Ni-rich cathode materials for lithium-ion batteries.

Keywords: Ni-rich NCM811 cathode; electron-conductive PDA-VGCFs filler; ion-conductive hybrid oligomer; lithium-ion batteries; surface modification.