Orientation-Engineered Anderson-Type Polyoxometalate Sub-1 nm Nanosheets for High-Performance Lithium-Ion Battery...

Area of Science:

• Materials Science
• Electrochemistry
• Nanotechnology

Background:

• Two-dimensional sub-1 nm nanosheets (2D SNSs) offer enhanced lithium-ion battery (LIB) performance due to short diffusion distances.
• Precise regulation of active sites on these nanosheets remains a significant challenge.

Purpose of the Study:

• To synthesize and characterize Zn-ZnMo6 sub-1 nm nanosheets (Zn-ZnMo6 SNSs) using a cluster self-assembly strategy.
• To investigate the relationship between active site exposure and electrochemical performance in LIB anodes.

Main Methods:

• Cluster self-assembly for synthesizing Zn-ZnMo6 SNSs.
• Molecular dynamics (MD) simulations to analyze stable configurations and active site exposure.
• Electrochemical testing (cycling performance, capacity) of LIB anodes.
• Density functional theory (DFT) calculations for adsorption energy analysis.

Main Results:

• Successfully synthesized Zn-ZnMo6 SNSs with two distinct configurations (Zn-ZnMo6-1 and Zn-ZnMo6-0.05).
• Zn-ZnMo6-1 exhibited exceptional LIB anode performance: 1361.9 mAh g⁻¹ capacity over 1500 cycles at 1 A g⁻¹.
• Zn-ZnMo6-1 significantly outperformed Zn-ZnMo6-0.05 (258.5 mAh g⁻¹).
• DFT revealed optimal lithium-ion adsorption at terminal-oxygen sites in Zn-ZnMo6-1 (Eads = -6.54 eV).

Conclusions:

• The cluster self-assembly strategy enables precise control over active site exposure in 2D SNSs.
• Zn-ZnMo6-1 demonstrates high capacity, excellent cycling stability, and redox reversibility for LIB anodes.
• This work presents a novel molecular-level approach for designing advanced 2D nanomaterials for energy storage applications.