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<p>The entangled electronic and geometric effects in heterogeneous catalysis have long obscured precise attribution of their individual roles. By employing a thermal-induced surface reconstruction strategy to progressively enhance metal-support interactions, we achieve continuous tuning of Pd’s electronic and geometric structures. Using alkyne semi-hydrogenation as a prototypical structure-sensitive probe reaction, we demonstrate that despite the linear coupling of electronic and geometric structures during Pd reconstruction, the turnover frequency scales solely with the geometric descriptor W (quantifying Pd particle flattening), while selectivity regulation bifurcates into two distinct regimes: Below a critical W, electron-deficient Pd sites offset geometric constraints, yielding a non-structure-sensitive selectivity plateau; whereas above this threshold, electron-rich surfaces establish unequivocal geometric control. Moreover, surface reconstruction drastically shrinks the electronic-geometric space of Pd sites for over-hydrogenation side reaction. These insights provide a blueprint for metal catalysts regulation in hydrogenation and may open avenues for quantifying electronic-geometric interplay in other structure-sensitive reactions.</p>

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Decoupling electronic and geometric effects in Pd catalysts via thermal surface reconstruction for selective hydrogenation

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月18日

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  • Minghang Li,
  • Zhaoyuan Fu,
  • Qian Luo,
  • Bing Lu,
  • Liwei Zhang,
  • Shipan Liang,
  • Ting Liu,
  • Yong Wang,
  • Shanjun Mao

摘要

The entangled electronic and geometric effects in heterogeneous catalysis have long obscured precise attribution of their individual roles. By employing a thermal-induced surface reconstruction strategy to progressively enhance metal-support interactions, we achieve continuous tuning of Pd’s electronic and geometric structures. Using alkyne semi-hydrogenation as a prototypical structure-sensitive probe reaction, we demonstrate that despite the linear coupling of electronic and geometric structures during Pd reconstruction, the turnover frequency scales solely with the geometric descriptor W (quantifying Pd particle flattening), while selectivity regulation bifurcates into two distinct regimes: Below a critical W, electron-deficient Pd sites offset geometric constraints, yielding a non-structure-sensitive selectivity plateau; whereas above this threshold, electron-rich surfaces establish unequivocal geometric control. Moreover, surface reconstruction drastically shrinks the electronic-geometric space of Pd sites for over-hydrogenation side reaction. These insights provide a blueprint for metal catalysts regulation in hydrogenation and may open avenues for quantifying electronic-geometric interplay in other structure-sensitive reactions.