Interfacial Engineering and a Low-Crystalline Strategy for High-Performance Supercapacitor Negative Electrodes: Fe₂P₂O₇ Nanoplates Anchored on N/P Co-doped Graphene Nanotubes

Developing novel hybrid negative electrode materials with high specific capacity, rate capacitance, and long-term cycle stability is a key factor for pushing large-scale application of supercapacitors. However, construction of robust interfaces and low-crystalline active materials plays a crucial role in realizing the target. In this paper, a one-step phosphorization approach was employed to make low-crystalline Fe2P2O7 nanoplates closely bonded to N/P-co-doped graphene nanotubes (N/P-GNTs@b-Fe2P2O7) through interfacial chemical bonding. The N and P heteroatoms as substitutions for C in GNT skeletons can introduce rich electronic centers, which induces Fe2P2O7 to fix the surface of N/P-GNTs through Fe–N and Fe–P bonds as confirmed by the characterizations. Moreover, the low-crystalline active materials own a disordered internal structure and numerous defects, which not only endows with excellent conductivity but also provides many active sites for redox reactions. Benefiting from the synergistic effects, the prepared N/P-GNTs@b-Fe2P2O7 can not only deliver a high capacity of 257 mA h g–1 (927 F g–1) at 1 A g–1 but also present an excellent rate capability of 184 mA h g–1 (665 F g–1) at 50 A g–1 and outstanding cycle stability (∼90.6% capacity retention over 40,000 cycles). Furthermore, an asymmetric supercapacitor was assembled using the obtained N/P-GNTs@b-Fe2P2O7 as electrode materials, which can present the energy density as high as 83.3 W h kg–1 at 791 W kg–1 and long-term durability. Therefore, this strategy not only offers an effective pathway for achieving high-performance negative electrode materials but also lays a foundation for further industrialization.