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<p>Achieving high ethylene selectivity while maintaining high activity in acetylene semi-hydrogenation over Pd-based catalysts remains a significant challenge. Herein, we report a Pd/g-C<sub>3</sub>N<sub>4</sub> catalyst with ultra-low Pd loading (0.05 wt%), synthesized via a facile chemical precipitation method, demonstrating enhanced catalytic performance. The strong metal-support interaction (SMSI) induced by pyridinic nitrogen species in g-C<sub>3</sub>N<sub>4</sub> stabilizes sub-nano Pd clusters. TPD analyses reveal that nanoparticle downsizing preferentially weakens ethylene adsorption by suppressing multi-site coordination (e.g., bridge/hollow configurations), thereby inhibiting over-hydrogenation. Concurrently, restricted hydrogen spillover in smaller Pd ensembles modulates hydrogen availability, achieving an optimal trade-off between acetylene conversion (100%) and ethylene selectivity (84.7%) at 55&#xa0;°C– the lowest operating temperature reported for Pd-based systems under similar conditions. This study proposes a particle size optimization strategy to modulate ethylene adsorption configurations and strength, thereby enhancing ethylene selectivity while establishing a paradigm for designing high-performance catalysts that reduce noble metal consumption without compromising industrial-grade performance.</p>

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High-Performance Pd/g-C3N4 Catalyst with Ultra-Low Pd Loading for Selective Hydrogenation of Acetylene in Excess Ethylene

  • 期刊论文

  • 发表日期：

    2025年8月9日

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  • Changjin Xu,
  • Jiuyang Wang,
  • Desheng Wang,
  • Herima Qi,
  • Riqing Cheng,
  • Jiahao Shi,
  • Wenyao Zhang,
  • Jianping Chen,
  • Huiqing Guo,
  • Junfang Ding

摘要

Achieving high ethylene selectivity while maintaining high activity in acetylene semi-hydrogenation over Pd-based catalysts remains a significant challenge. Herein, we report a Pd/g-C3N4 catalyst with ultra-low Pd loading (0.05 wt%), synthesized via a facile chemical precipitation method, demonstrating enhanced catalytic performance. The strong metal-support interaction (SMSI) induced by pyridinic nitrogen species in g-C3N4 stabilizes sub-nano Pd clusters. TPD analyses reveal that nanoparticle downsizing preferentially weakens ethylene adsorption by suppressing multi-site coordination (e.g., bridge/hollow configurations), thereby inhibiting over-hydrogenation. Concurrently, restricted hydrogen spillover in smaller Pd ensembles modulates hydrogen availability, achieving an optimal trade-off between acetylene conversion (100%) and ethylene selectivity (84.7%) at 55 °C– the lowest operating temperature reported for Pd-based systems under similar conditions. This study proposes a particle size optimization strategy to modulate ethylene adsorption configurations and strength, thereby enhancing ethylene selectivity while establishing a paradigm for designing high-performance catalysts that reduce noble metal consumption without compromising industrial-grade performance.