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<p>Pd catalysts demonstrate remarkable activity and selectivity for the direct oxidation methane-to-methanol (DOMM) under mild conditions. However, understanding the structure–performance relationship is challenging because Pd catalysts used in existing studies have complex polycrystalline structures. In this work, well-defined Pd nanocrystals with controlled morphologies are synthesized and used as model systems to investigate the origins of the observed structure-activity differences. Our findings indicate that DOMM activity is primarily governed by crystal facet type rather than nanocrystal size. The lower <i>d</i>-band center of the Pd {111} facet weakens the adsorption strength of critical intermediates, including *O<sub>2</sub> and *OH species, promoting H<sub>2</sub>O<sub>2</sub> generation and CH<sub>3</sub>OH formation, respectively. Consequently, {111}-dominated octahedral Pd nanocrystals achieve an exceptional CH<sub>3</sub>OH yield of 201.8 mmol·g<sub>Pd</sub><sup>−1</sup>·h<sup>−1</sup>, three times higher than that of their {100}-dominated hexahedral counterparts. These results provide key insights into the structure-dependent behavior of Pd catalysts and pave the way for designing high-performance catalysts for DOMM.</p>

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Pd nanocatalysts engineering for direct oxidation methane-to-methanol with 99.7% selectivity

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年8月19日

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  • Peilin Deng,
  • Yueshan Xu,
  • Daoxiong Wu,
  • Ying Liang,
  • Xue Zhang,
  • Zhitong Wang,
  • Jing Li,
  • Xinlong Tian

摘要

Pd catalysts demonstrate remarkable activity and selectivity for the direct oxidation methane-to-methanol (DOMM) under mild conditions. However, understanding the structure–performance relationship is challenging because Pd catalysts used in existing studies have complex polycrystalline structures. In this work, well-defined Pd nanocrystals with controlled morphologies are synthesized and used as model systems to investigate the origins of the observed structure-activity differences. Our findings indicate that DOMM activity is primarily governed by crystal facet type rather than nanocrystal size. The lower d-band center of the Pd {111} facet weakens the adsorption strength of critical intermediates, including *O2 and *OH species, promoting H2O2 generation and CH3OH formation, respectively. Consequently, {111}-dominated octahedral Pd nanocrystals achieve an exceptional CH3OH yield of 201.8 mmol·gPd−1·h−1, three times higher than that of their {100}-dominated hexahedral counterparts. These results provide key insights into the structure-dependent behavior of Pd catalysts and pave the way for designing high-performance catalysts for DOMM.