Self‐Crosslinked Poly(acrylonitrile‐co‐acrylamide) for Carbon Nanofibers With Improved Mechanical Performance and Structural Integrity

ABSTRACT This study reports a novel approach to significantly enhance the mechanical performance and structural integrity of carbon nanofibers (CNFs) through self‐crosslinked poly(acrylonitrile‐co‐acrylamide) P(AN‐AM) copolymers. P(AN‐AM) undergoes self‐crosslinking to form a stable, continuous covalent network that effectively dissipates stress during thermal stabilization and carbonization, reducing the risk of fiber fracture. Concurrently, the transformation of nitrile groups into imine groups lowers the activation barrier for radical‐mediated cyclization, promoting the formation of ladder‐like structures and optimizing the stabilization process at the molecular level. Simultaneously, the crosslinked network further restricts polymer chain mobility, facilitating ladder‐like structures formation. The resulting CNFs retain high structural integrity and exhibit enhanced internal graphitic ordering, achieving a tensile strength of 26.66 ± 2.11 MPa. These findings establish self‐crosslinked P(AN‐AM) as a scalable and effective strategy for producing high‐performance CNFs for advanced structural and functional applications.