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<p>Integrating metals and polymers is pivotal for advanced functional applications, yet their intrinsic electronic bonding origin remains elusive due to material mismatch. Combining density functional theory (DFT) calculations and experiments, this study establishes a unified interfacial electron donor-acceptor framework. We demonstrate that interfacial metal oxides and polymer carboxyl groups facilitate <i>μ</i>₂-bridging coordination, driven by <i>p</i>-<i>p</i> σ hybridization between metal vacant 3<i>p</i> and oxygen lone-pair 2<i>p</i> orbitals, which is verified by valence band spectra. Furthermore, introducing surface oxygen vacancies enhances the electron-accepting capability of metal sites, enabling the coordinated interface to resist thermodynamic fluctuations, thereby improving the tensile-shear strength by over 400%. Cross-system validations across various cation valence states (+1 to +4) and polymer heteroatoms successfully demonstrate the general applicability of this theory-guided acceptor mechanism among diverse structural alloys and thermoplastics. This work provides a predictive electronic-structure foundation for the rational design of high-performance multi-material hybrid interfaces beyond specific systems.</p>

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Elucidation of the intrinsic electronic mechanism governing interfacial chemical bonding in metal-polymer hybrids

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年7月23日

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  • Yifan Liu,
  • Jianhui Su,
  • Ri Han,
  • Jiaheng Zhang,
  • Fuyun Liu,
  • Caiwang Tan,
  • Swee Leong Sing,
  • Xiaohui Han,
  • Bo Chen,
  • Xiaoguo Song

摘要

Integrating metals and polymers is pivotal for advanced functional applications, yet their intrinsic electronic bonding origin remains elusive due to material mismatch. Combining density functional theory (DFT) calculations and experiments, this study establishes a unified interfacial electron donor-acceptor framework. We demonstrate that interfacial metal oxides and polymer carboxyl groups facilitate μ₂-bridging coordination, driven by p-p σ hybridization between metal vacant 3p and oxygen lone-pair 2p orbitals, which is verified by valence band spectra. Furthermore, introducing surface oxygen vacancies enhances the electron-accepting capability of metal sites, enabling the coordinated interface to resist thermodynamic fluctuations, thereby improving the tensile-shear strength by over 400%. Cross-system validations across various cation valence states (+1 to +4) and polymer heteroatoms successfully demonstrate the general applicability of this theory-guided acceptor mechanism among diverse structural alloys and thermoplastics. This work provides a predictive electronic-structure foundation for the rational design of high-performance multi-material hybrid interfaces beyond specific systems.