Low-dimensional sp²-based carbon nanostructures, known for their remarkable transport properties and mechanical behaviors, are widely used as reinforcing phases in polymer composites to enhance their performance. While carbon nanocomposites are promising materials for extreme conditions, the damage mechanisms due to charge injection at the interfaces between carbon nanostructures and polymers remain unclear. Using first-principles calculations, we investigated ambipolar charging and structural responses at the interfaces between industrially relevant polymers and carbon nanotubes or graphene upon electron and hole injection. Our electronic structure analysis reveals that resistance to charge injection is closely related to the band structures of the polymers and the chemistry of interfacial cross-links. Mechanical behaviors assessed through traction and shear tests reflect changes in electronic coupling at the interfaces. Our results indicate significantly degraded mechanical performance with electron injection, while slight hole injection leads to shortening and stiffening of covalent bonds. These findings provide crucial insights for the design of carbon nanocomposites intended for harsh environments, such as lightning strikes and high-power electromagnetic shocks.

中文翻译：

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纳米级界面的双极充电响应


低维 sp² 基碳纳米结构以其卓越的传输性能和机械行为而闻名，被广泛用作聚合物复合材料中的增强相以提高其性能。虽然碳纳米复合材料是适用于极端条件的有前途的材料，但在碳纳米结构和聚合物之间的界面处注入电荷引起的损伤机制仍不清楚。使用第一性原理计算，我们研究了电子和空穴注入后工业相关聚合物与碳纳米管或石墨烯之间界面的双极电荷和结构响应。我们的电子结构分析表明，抗电荷注入与聚合物的能带结构和界面交联的化学性质密切相关。通过牵引和剪切测试评估的机械行为反映了界面处电子耦合的变化。我们的结果表明，电子注入的机械性能显着下降，而轻微的空穴注入会导致共价键的缩短和变硬。这些发现为设计用于恶劣环境（如雷击和高功率电磁冲击）的碳纳米复合材料的设计提供了重要的见解。