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

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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 freestanding 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.

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Acknowledgements

H. F. acknowledges financial support from the National Natural Science Foundation of China (No. 51902099), Hunan high-level talent gathering project (No. 2019RS1021), Fundamental Research Funds for the Central Universities (No. 531119200087).

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  1. 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

    Lingli Xing, Rui Liu, Zhichao Gong, Jingjing Liu, Jianbin Liu, Haisheng Gong, Kang Huang & Huilong Fei

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  1. Lingli Xing
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Xing, L., Liu, R., Gong, Z. et al. Ultrafast Joule heating synthesis of hierarchically porous graphene-based Co-N-C single-atom monoliths. Nano Res. 15, 3913–3919 (2022). https://doi.org/10.1007/s12274-021-4046-z

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