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Research Article

Ultrafast Joule heating synthesis of hierarchically porous graphene-based Co-N-C single-atom monoliths

Lingli Xing, Rui Liu, Zhichao Gong, Jingjing Liu, Jianbin Liu, Haisheng Gong, Kang Huang, Huilong Fei ( )
Advanced Catalytic Engineering Research Center of the Ministry of Education, State Key Laboratory for Chemo/Biosensing and Chemometrics, and College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China
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Graphical Abstract

The ultrafast Joule heating process ensures the rapid and stable dispersion of atomic-scale CoNx active sites in graphene, while the three-dimensional hierarchically porous architecture promotes the mass transfer efficiency during the catalytic process.

Abstract

Herein, we develop a transient heating-quenching strategy triggered by Joule heating for the synthesis of single-atom cobalt- and nitrogen-doped graphene materials with three-dimensional porous monolithic architecture (denoted as CoNG-JH). The ultrafast Joule heating procedure simultaneously enables the reduction of graphene oxide and the incorporation of metal and nitrogen atoms into the graphene matrix within 2-second period. Meanwhile, the transient quenching avoids the extended heating-induced atom aggregation, ensuring the rapid and stable dispersion of atomic-scale CoNx active sites in graphene. Additionally, the interconnected macropores and nanopores formed by the self-assembly of graphene sheets facilitate the unimpeded ion and gas transport during the catalytic process. When used as an electrode for the hydrogen evolution reaction (HER), the fabricated free-standing CoNG-JH exhibits high catalytic activity and durability with a low overpotential of 106 mV at 10 mA·cm−2 and a small Tafel slope of 66 mV·dec−1 in 0.5 M H2SO4 electrolyte. The presented synthesis and design strategy open up a rapid and facile route for the manufacturing of single atom catalysts.

Keywords

Joule heatingsingle atom catalystshierarchically porous structureself-supporting filmhydrogen evolution reaction

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Nano Research
Volume 15 Issue 5,
May 2022
Pages 3913-3919
DOI: 10.1007/s12274-021-4046-z
Cite this article:
Xing L, Liu R, Gong Z, et al. Ultrafast Joule heating synthesis of hierarchically porous graphene-based Co-N-C single-atom monoliths. Nano Research, 2022, 15(5): 3913-3919. https://doi.org/10.1007/s12274-021-4046-z
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Received: 06 November 2021
Revised: 02 December 2021
Accepted: 04 December 2021
Published: 31 December 2021
© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021
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