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<p>Alkali metals have been widely used as promoters in heterogeneous metal catalysts to improve activity, product selectivity, and stability. Despite their prevalence, the precise role remains not fully uncovered due to the complex interplay between catalytic components and reactants involving dynamic structural changes. Herein, we elucidate the promotional effect of alkali metal in hydrogenation reactions from a unified perspective. Using Na-doped Rh/TiO<sub>2</sub> as a representative system, we demonstrate a phenomenon, termed “Strong Metal–Base Interaction (SMBI)”. The basic Na species (e.g. Na<sub>2</sub>O) intimate to the Rh particles facilitates heterolytic H<sub>2</sub> splitting, capturing H<sup>+</sup> while leaving H<sup>−</sup> on Rh sites. Consequently, there are suppressed hydrogen spillovers from Rh to the TiO<sub>2</sub> surface and electron-rich Rh sites, fundamentally altering the catalytic behavior during hydrogenation. SMBI enables fine control of both activity and selectivity: Na doping shifts product selectivity in CO<sub>2</sub> hydrogenation completely from CH<sub>4</sub> to CO, enhances C=C hydrogenation via weakened H adsorption and electron-enriched Rh, and suppresses C=O and N=O hydrogenation due to restricted H spillover. These findings provide a unified framework for understanding alkali metal promotion and offer a rational approach for designing efficient hydrogenation catalysts.</p>

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Understanding alkali metal promotion in hydrogenation catalysis through Strong Metal–Base Interaction

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月30日

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  • Munam Jung,
  • Maxim Park Dickieson,
  • Pinzhang Chen,
  • Clemen Jia Gen Goh,
  • Peijie Han,
  • Bingqing Yao,
  • Xing-Chi Li,
  • Haruya Hattori,
  • Qian He,
  • Ya-Wen Zhang,
  • Kyungho Lee,
  • Ning Yan

摘要

Alkali metals have been widely used as promoters in heterogeneous metal catalysts to improve activity, product selectivity, and stability. Despite their prevalence, the precise role remains not fully uncovered due to the complex interplay between catalytic components and reactants involving dynamic structural changes. Herein, we elucidate the promotional effect of alkali metal in hydrogenation reactions from a unified perspective. Using Na-doped Rh/TiO2 as a representative system, we demonstrate a phenomenon, termed “Strong Metal–Base Interaction (SMBI)”. The basic Na species (e.g. Na2O) intimate to the Rh particles facilitates heterolytic H2 splitting, capturing H+ while leaving H− on Rh sites. Consequently, there are suppressed hydrogen spillovers from Rh to the TiO2 surface and electron-rich Rh sites, fundamentally altering the catalytic behavior during hydrogenation. SMBI enables fine control of both activity and selectivity: Na doping shifts product selectivity in CO2 hydrogenation completely from CH4 to CO, enhances C=C hydrogenation via weakened H adsorption and electron-enriched Rh, and suppresses C=O and N=O hydrogenation due to restricted H spillover. These findings provide a unified framework for understanding alkali metal promotion and offer a rational approach for designing efficient hydrogenation catalysts.