Dynamic Microinterfacial Polymerization Enables Scalable Synthesis of Two-Dimensional Polymer Sheets for...

Area of Science:

• Materials Science
• Polymer Chemistry
• Electrochemistry

Background:

• Organic two-dimensional (2D) materials offer vast application potential but face limitations in structural diversity and synthesis.
• Developing novel 2D materials with scalable synthetic routes is crucial for advancing technologies.

Purpose of the Study:

• To synthesize novel 2D polymer sheets using a dynamic microinterfacial polymerization method.
• To create sodium-ion conducting materials and composite membranes for quasi-solid-state electrolytes (QSSE).
• To evaluate the performance of the QSSE in sodium-ion cells.

Main Methods:

• Dynamic microinterfacial polymerization of poly(propylene glycol)bis(2-aminopropyl ether) and 1,3,5-benzenetricarbonyl trichloride to form 2D polymer sheets (PEO-BTA).
• Conversion of PEO-BTA sheets to Na-ion conducting materials using sodium hydride.
• Incorporation of a metal-organic framework (MOF, HKUST-1) to form composite sheets (MOF@PEO-BTA-Na).
• Assembly of composite sheets into self-supporting membranes for QSSE applications.

Main Results:

• Successfully synthesized novel 2D polymer sheets (PEO-BTA) via a scalable microinterfacial polymerization.
• Developed Na-ion conducting composite sheets (MOF@PEO-BTA-Na) with structural integrity.
• Achieved high ionic conductivity (2.80 × 10^-3 S cm^-1) and Na⁺ transference number (0.95) for the QSSE.
• Demonstrated uniform Na plating and excellent electrochemical performance in Na//Na and Na//NaTi₂(PO₄)₃ cells, including high capacity retention (92% after 1000 cycles).

Conclusions:

• Established a new, scalable synthetic approach for 2D organic sheets.
• Demonstrated the potential of MOF@PEO-BTA-Na composite sheets as high-performance QSSEs for sodium-ion batteries.
• Highlighted the promising applications of these novel 2D materials in energy storage devices.