Fullerene‐Derived Porous and Defective N‐Doped Carbon Nanosheets as Advanced Trifunctional Metal‐Free Electrocatalysts
Zhimin He, Ziwei Zhou, Peng Wei, Ting Xu, Jiantao Han, Keke Huang, Kun Guo, Wenhuan Huang, Takeshi Akasaka, Xing Lü
Abstract
Abstract Dopants and defects are crucial for multifunctional carbon‐based metal‐free electrocatalysts, but the rational design and facile production remain as a big challenge. Herein, we report a novel strategy using salt‐assisted pyrolysis of derivatized fullerenes to fabricate defect‐rich and N‐doped carbon nanosheets. Molecular level modification of C 60 via amination and hydroxylation gives rise to well‐defined fullerol molecules bearing N‐containing groups (FNG). Subsequent calcination of FNG and NaCl at 750 °C generates porous carbon nanosheets (FNCNs‐750) and turns the N‐containing groups into high‐level N dopants (12.43 at.%). Further pyrolysis of FNCNs‐750 at 900 °C (FNCNs‐900) leads to a reduced N content populated by graphitic‐N. Meanwhile, abundant intrinsic defects (e. g., topological defects and edges) are created due to the breakdown of fullerene cages and partial removal of edged N atoms. These structural features endow FNCNs‐900 with outstanding trifunctional catalytic performance, better than or close to the noble metal‐based benchmark catalysts.