Strong metal oxide-support interaction in MoO2/N-doped MCNTs heterostructure for boosting lithium storage performance

Zhicheng Wang; Xing Chen; Dajun Wu; Tao Zhang; Guikai Zhang; Shengqi Chu; Bin Qian; Shi Tao

doi:10.1016/j.jcis.2023.06.192

Strong metal oxide-support interaction in MoO₂/N-doped MCNTs heterostructure for boosting lithium storage performance

J Colloid Interface Sci. 2023 Nov 15;650(Pt A):247-256. doi: 10.1016/j.jcis.2023.06.192. Epub 2023 Jun 28.

Authors

Zhicheng Wang¹, Xing Chen², Dajun Wu¹, Tao Zhang³, Guikai Zhang⁴, Shengqi Chu⁴, Bin Qian¹, Shi Tao⁵

Affiliations

¹ School of Electronic and Information Engineering, Jiangsu Laboratory of Advanced Functional Materials, Changshu Institute of Technology, Changshu 215500, China.
² Institutes of Physical Science and Information Technology, Anhui University, Hefei 230601, China.
³ School of Physical and Mathematical Sciences, Nanyang Technological University, 21 Nanyang Link, Singapore 637371, Singapore. Electronic address: tao.zhang@ntu.edu.sg.
⁴ Beijing Synchrotron Radiation Facility, Institute of High Energy Physics Chinese Academy of Sciences, Beijing 100049, China.
⁵ School of Electronic and Information Engineering, Jiangsu Laboratory of Advanced Functional Materials, Changshu Institute of Technology, Changshu 215500, China. Electronic address: taoshi@cslg.edu.cn.

PMID: 37406565
DOI: 10.1016/j.jcis.2023.06.192

Abstract

The low-rate capability and fast capacity decaying of the molybdenum dioxide anode material have been a bottleneck for lithium-ion batteries (LIBs) due to low carrier transport, drastic volume expansion and inferior reversibility. Furthermore, the lithium-storage mechanism is still controversial at present. Herein, we fabricate a new kind of MoO₂ nanoparticles with nitrogen-doped multiwalled carbon nanotubes (MoO₂/N-MCNTs) as anode for LIBs. The strong chemical bonding (MoOC) endows MoO₂/N-MCNTs a strong metal oxide-support interaction (SMSI), rendering electron/ion transfer and facilitate significant Li⁺ intercalation pseudocapacitance, which is evidenced by both theoretical computation and detailed experiments. Thus, the MoO₂/N-MCNTs exhibits high-rate performance (523.7 mAh/g at 3000 mA g^-1) and long durability (507.8 mAh/g at 1000 mA g^-1 after 500 cycles). Furthermore, pouch-type full cell composed of MoO₂/N-MCNTs anodes and commercial LiNi_0.6Co_0.2Mn_0.2O₂ (NCM622) cathodes demonstrate impressive rate performance and cyclic life, which displays an unparalleled energy density of 553.0 Wh kg^-1. Ex-situ X-ray absorption spectroscopy (XAS) indicates the enhanced lithium-storage mechanism is originated from a partially irreversible phase transition from Li_0.98MoO₂ to Li₂MoO₄ via delithiation. This work not only provides fresh insights into the enhanced lithium-storage mechanism but also proposes new design principles toward efficient LIBs.

Keywords: Carbon nanotubes; Lithium-storage mechanism; Molybdenum dioxide; Strong metal oxide–support interaction; X-ray absorption spectroscopy.