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<p>Acetylene semihydrogenation is a critical process in the polyolefin industry by selectively removing trace acetylene from ethylene-rich reformate. However, this reaction is generally limited by the inherent activity-selectivity trade-off due to the thermodynamic advantage of overhydrogenation. Herein, we develop a facile and straightforward strategy to construct Pd<sub>2</sub> dual-atom sites anchored on defect-rich surface-graphitized nanodiamond (ND@G) via the solvent-mediated dispersion of palladium carboxylate driven by the chelation of palladium precursors via carboxylate anion. Cs-corrected HAADF-STEM images coupled with XAS analysis unambiguously manifest the successful architecting of Pd<sub>2</sub> dual-atom sites. Compared to Pd<sub>1</sub> single-atom sites, the obtained Pd<sub>2</sub>/ND@G sample demonstrates superior catalytic performance in acetylene semihydrogenation, with the corresponding TOF values increased from 0.151 s<sup>−1</sup> to 1.953 s<sup>−1</sup>, without the obvious decline of ethylene selectivity (93.2%, at full acetylene conversion). C<sub>2</sub>H<sub>2</sub>/C<sub>2</sub>H<sub>4</sub>-TPD, H<sub>2</sub>-D<sub>2</sub> exchange reaction, isotope-labeled TPSR combined with DFT calculations confirm the effective co-activation of C<sub>2</sub>H<sub>2</sub>/H<sub>2</sub> on Pd<sub>2</sub> dual-atom sites while maintaining the weak adsorption of ethylene similar to that on its single-atom sites, which can break the activity-selectivity trade-off in acetylene semihydrogenation.</p>

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Breaking the activity-selectivity trade-off for acetylene semihydrogenation by Pd2 dual-atom site

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月25日

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  • Feng Hong,
  • Hongqiu Chen,
  • Jiawei Chen,
  • Zhehan Ying,
  • Mi Peng,
  • Jingwang Zhang,
  • Zuodong Yang,
  • Guodong Wen,
  • Jiangyong Diao,
  • Bo Sun,
  • Geng Sun,
  • Ding Ma,
  • Hongyang Liu

摘要

Acetylene semihydrogenation is a critical process in the polyolefin industry by selectively removing trace acetylene from ethylene-rich reformate. However, this reaction is generally limited by the inherent activity-selectivity trade-off due to the thermodynamic advantage of overhydrogenation. Herein, we develop a facile and straightforward strategy to construct Pd2 dual-atom sites anchored on defect-rich surface-graphitized nanodiamond (ND@G) via the solvent-mediated dispersion of palladium carboxylate driven by the chelation of palladium precursors via carboxylate anion. Cs-corrected HAADF-STEM images coupled with XAS analysis unambiguously manifest the successful architecting of Pd2 dual-atom sites. Compared to Pd1 single-atom sites, the obtained Pd2/ND@G sample demonstrates superior catalytic performance in acetylene semihydrogenation, with the corresponding TOF values increased from 0.151 s−1 to 1.953 s−1, without the obvious decline of ethylene selectivity (93.2%, at full acetylene conversion). C2H2/C2H4-TPD, H2-D2 exchange reaction, isotope-labeled TPSR combined with DFT calculations confirm the effective co-activation of C2H2/H2 on Pd2 dual-atom sites while maintaining the weak adsorption of ethylene similar to that on its single-atom sites, which can break the activity-selectivity trade-off in acetylene semihydrogenation.