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<p>Waterborne polyurethane (WPU) has garnered significant interest due to its excellent mechanical properties, chemical stability, and structural tunability. Its application in silicon-based anodes for lithium-ion batteries (LIBs) is particularly promising for mitigating the severe volume expansion of silicon and the consequent deterioration of electrode stability during cycling. In this study, a series of poly (methyl methacrylate)-modified waterborne polyurethane (WPUA) adhesives were synthesized by first preparing a waterborne polyurethane with hydroxyethyl acrylate (HEA) as the terminal group, followed by copolymerization with methyl methacrylate (MMA). The effects of the PMMA/WPU mass ratio on the structural, mechanical, and electrochemical properties were systematically investigated. Fourier Transform Infrared (FTIR), Thermogravimetric Analysis (TGA), and Differential Scanning Calorimetry (DSC) analyses revealed that the incorporation of MMA increased the polymer molecular weight, cross-linking density, and chain rigidity, thereby improving the interfacial adhesion to both the copper foil and active materials. The modified binder synergistically combines the flexibility of WPU with the rigidity of PMMA, effectively buffering the stress generated from the volume variation of silicon anodes and maintaining electrode integrity. The optimized WPUA3 sample (with a WPU/PMMA mass ratio of 7:3) demonstrated superior performance: a tensile strength of 8.28&#xa0;MPa, an average peeling force of 0.92&#xa0;N, an initial discharge specific capacity of 912 mAh·g⁻¹ with a Coulombic efficiency of 95.88%, a capacity retention of 82.57% after 100 cycles, and a reversible capacity of 192 mAh·g⁻¹ at a 5&#xa0;C rate. These results confirm that MMA-modified WPU binders can significantly enhance the adhesion and cycling stability of silicon-based anodes, offering a promising solution for high-performance lithium-ion batteries.</p>

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Synthesis of methyl methacrylate-modified waterborne polyurethane and its application in lithium-ion batteries

  • 期刊论文

  • 发表日期：

    2026年3月23日

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  • Tao Jin,
  • Zhen-xiang Guan,
  • Hai-jun Kou,
  • Jia-jia Wu,
  • Yun-dong Ji,
  • Li-li Wu

摘要

Waterborne polyurethane (WPU) has garnered significant interest due to its excellent mechanical properties, chemical stability, and structural tunability. Its application in silicon-based anodes for lithium-ion batteries (LIBs) is particularly promising for mitigating the severe volume expansion of silicon and the consequent deterioration of electrode stability during cycling. In this study, a series of poly (methyl methacrylate)-modified waterborne polyurethane (WPUA) adhesives were synthesized by first preparing a waterborne polyurethane with hydroxyethyl acrylate (HEA) as the terminal group, followed by copolymerization with methyl methacrylate (MMA). The effects of the PMMA/WPU mass ratio on the structural, mechanical, and electrochemical properties were systematically investigated. Fourier Transform Infrared (FTIR), Thermogravimetric Analysis (TGA), and Differential Scanning Calorimetry (DSC) analyses revealed that the incorporation of MMA increased the polymer molecular weight, cross-linking density, and chain rigidity, thereby improving the interfacial adhesion to both the copper foil and active materials. The modified binder synergistically combines the flexibility of WPU with the rigidity of PMMA, effectively buffering the stress generated from the volume variation of silicon anodes and maintaining electrode integrity. The optimized WPUA3 sample (with a WPU/PMMA mass ratio of 7:3) demonstrated superior performance: a tensile strength of 8.28 MPa, an average peeling force of 0.92 N, an initial discharge specific capacity of 912 mAh·g⁻¹ with a Coulombic efficiency of 95.88%, a capacity retention of 82.57% after 100 cycles, and a reversible capacity of 192 mAh·g⁻¹ at a 5 C rate. These results confirm that MMA-modified WPU binders can significantly enhance the adhesion and cycling stability of silicon-based anodes, offering a promising solution for high-performance lithium-ion batteries.