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Fullerene-Derived Porous and Defective N-Doped Carbon Nanosheets as Advanced Trifunctional Metal-Free Electrocatalysts |
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| Authors: | Dr Zhimin He Ziwei Zhou Dr Peng Wei Dr Ting Xu Prof Jiantao Han Prof Keke Huang Dr Kun Guo Prof Wenhuan Huang Prof Takeshi Akasaka Prof Xing Lu |
| Institution: | 1. State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, 430074 P. R. China
These authors contributed equally to this work.;2. State Key Laboratory of Inorganic Synthesis & Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P. R. China These authors contributed equally to this work.;3. State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, 430074 P. R. China;4. State Key Laboratory of Inorganic Synthesis & Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P. R. China;5. Shaanxi Key Laboratory of Chemical Additives for Industry, College of Chemistry & Chemical Engineering, Shaanxi University of Science & Technology, Xi'an, 710021 P. R. China |
| 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 C60 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. |
| Keywords: | fullerene N dopants structural defects metal-free carbon trifunctional electrocatalysts |