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<p>Supported noble metal catalysts are central to industrial, environmental, and energy applications, yet precisely constructing active sites with optimized geometry remains a formidable challenge beyond conventional particle size control. Here, we introduce a perovskite-based surface defect engineering strategy that enables atomic-level regulation of noble metal active sites. By tailoring La stoichiometry in LaAlO<sub>3</sub>, we engineer three distinct surface morphologies (planar, stepped, and crater-like) that serve as templates for anchoring and replicating supported PdO nanoparticles. Among these, the step-rich PdO configuration on La<sub>0.9</sub>AlO<sub>3−δ</sub> exhibits the highest methane oxidation activity, with a linear correlation between Pd step-site density and catalytic performance. The enhancement arises from low-coordination Pd atoms at step sites, which form stable Pd–C(CH<sub>3</sub>) covalent bonds and facilitate C–H bond activation, the rate-determining step in methane oxidation. This work establishes a generalizable approach to precisely tailor noble metal active sites through perovskite surface engineering, providing a robust framework for the rational design of efficient and durable oxidation catalysts.</p>

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Defect-engineered nonstoichiometric perovskite hosting high-activity PdO sites for enhanced hydrocarbon oxidation

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年4月2日

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  • Jihang Yu,
  • Zhi-Qiang Wang,
  • Yongjun Jiang,
  • Jiaorong Yan,
  • Yanglong Guo,
  • Yun Guo,
  • Li Wang,
  • Aiyong Wang,
  • Sheng Dai,
  • Feng Gao,
  • Wangcheng Zhan

摘要

Supported noble metal catalysts are central to industrial, environmental, and energy applications, yet precisely constructing active sites with optimized geometry remains a formidable challenge beyond conventional particle size control. Here, we introduce a perovskite-based surface defect engineering strategy that enables atomic-level regulation of noble metal active sites. By tailoring La stoichiometry in LaAlO3, we engineer three distinct surface morphologies (planar, stepped, and crater-like) that serve as templates for anchoring and replicating supported PdO nanoparticles. Among these, the step-rich PdO configuration on La0.9AlO3−δ exhibits the highest methane oxidation activity, with a linear correlation between Pd step-site density and catalytic performance. The enhancement arises from low-coordination Pd atoms at step sites, which form stable Pd–C(CH3) covalent bonds and facilitate C–H bond activation, the rate-determining step in methane oxidation. This work establishes a generalizable approach to precisely tailor noble metal active sites through perovskite surface engineering, providing a robust framework for the rational design of efficient and durable oxidation catalysts.