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Ethane dehydrogenation over the g-C3N4 supported metal single-atom catalysts to enhance reactivity and coking-resistance ability

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Abstract

Ethane dehydrogenation (EDH) to produce ethylene requires high operating temperature to achieve satisfactory ethylene yield, however, this process leads to coke formation and catalyst deactivation. Here, an active site isolation strategy was employed to inhibit side reaction and coke formation over fifteen types of metal single-atom metal/graphitic carbon nitride (M/g-C3N4) catalysts. Density functional theory (DFT) calculations completely describe reaction network of ethane dehydrogenation. On-lattice kinetic Monte Carlo simulations were carried out to evaluate catalytic performance under the realistic conditions. The Co/g-C3N4, Rh/g-C3N4, and Ni/g-C3N4 catalysts were screened out to exhibit higher C2H4(g) formation activity and C2H4(g) selectivity close to or equal to 100%. The low reactant partial pressure 0%–5% at atmospheric pressure facilitates ethane dehydrogenation, and the appropriate temperatures over Co/g-C3N4, Rh/g-C3N4, and Ni/g-C3N4 catalysts are 673.15, 723.15, and 723.15 K, respectively. Especially, Co/g-C3N4 catalyst presents the highest C2H4(g) formation activity, attributing to the appropriate anti-bonding strength between C atom and metal single-atom. Further, a simple descriptor, the reaction energy of C2H5* dehydrogenation to C2H4*, was proposed to quantitatively and quickly evaluate C2H4(g) formation activity. The present study laid a solid foundation for efficient design and development of single-atom catalysts with high-performance for selective dehydrogenation of alkanes.

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Acknowledgments

This work is financially supported by the National Key R&D Program of China (No. 2021YFA1502804), the National Natural Science Foundation of China (Nos. 22078221 and 21776193), and the Science Foundation for Distinguished Young Scholar of Shanxi Province (No. 20210302121005).

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Authors and Affiliations

  1. College of Chemical Engineering and Technology, Taiyuan University of Technology, Taiyuan, 030024, China

    Yuan Zhang, Baojun Wang & Lixia Ling

  2. State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan, 030024, China

    Yuan Zhang, Baojun Wang, Lixia Ling & Riguang Zhang

  3. Departments of Chemical and Petroleum Engineering, University of Wyoming, Laramie, WY, 82071, USA

    Maohong Fan

  4. School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, GA, 30332, USA

    Maohong Fan

  5. School of Energy Resources, University of Wyoming, Laramie, WY, 82071, USA

    Maohong Fan

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  1. Yuan Zhang
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  2. Baojun Wang
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  4. Lixia Ling
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  5. Riguang Zhang
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Correspondence to Baojun Wang or Riguang Zhang.

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Ethane dehydrogenation over the g-C3N4 supported metal single-atom catalysts to enhance reactivity and coking-resistance ability

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Zhang, Y., Wang, B., Fan, M. et al. Ethane dehydrogenation over the g-C3N4 supported metal single-atom catalysts to enhance reactivity and coking-resistance ability. Nano Res. 16, 6142–6152 (2023). https://doi.org/10.1007/s12274-022-5187-4

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