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<p>Despite the growing significance of adsorbate-mediated strong metal-support interaction (A-SMSI) in various catalytic processes, a comprehensive mechanistic understanding of its formation and effective strategies for its precise modulation remain elusive. Herein, by constructing three well-defined model Ni/TiO<sub>2</sub> catalysts with distinct exposed facets, we directly visualize a facet-dependent A-SMSI behavior in CO<sub>2</sub> hydrogenation via in situ environmental transmission electron microscopy (ETEM) at the atomic level. The in situ results reveal distinct formation behaviors of TiO<sub>2-x</sub> overlayers: complete, partial, and no encapsulation of Ni nanoparticles (NPs) on the {100}, {101}, and {001} TiO<sub>2</sub> facets, respectively. Complementary in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), X-ray absorption spectroscopy (XAS) experiments and density functional theory (DFT) calculations further reveal a dual induction mechanism, where adsorbates both participate in TiO<sub>2-x</sub> formation and stabilize the encapsulating overlayer. Moreover, TiO<sub>2-x</sub> transfers electrons to Ni and stabilizes COOH<sup>*</sup> intermediates that dehydroxylate to form CO. Guided by these mechanistic insights, facet-dependent A-SMSI enables remarkable selectivity modulation, yielding CH<sub>4</sub> selectivity exceeding 88% on Ni/TiO<sub>2</sub>-{001} and CO selectivity over 83% on Ni/TiO<sub>2</sub>-{100}. These findings advance the fundamental understanding of A-SMSI and offer a rational framework for designing oxide-supported catalysts with tailored interfacial properties.</p>

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Facet-dependent adsorbate-mediated strong metal-support interaction in Ni/TiO2

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月18日

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  • Liboting Gao,
  • Hao Zhang,
  • Yanhui Long,
  • Fangwen Yang,
  • Zijiang Zhao,
  • Zhongkang Han,
  • Rui Tang,
  • Yilin Zhang,
  • Xiaosong An,
  • Xiaodong Li,
  • Wentao Yuan,
  • Yong Wang,
  • Jianhua Yan

摘要

Despite the growing significance of adsorbate-mediated strong metal-support interaction (A-SMSI) in various catalytic processes, a comprehensive mechanistic understanding of its formation and effective strategies for its precise modulation remain elusive. Herein, by constructing three well-defined model Ni/TiO2 catalysts with distinct exposed facets, we directly visualize a facet-dependent A-SMSI behavior in CO2 hydrogenation via in situ environmental transmission electron microscopy (ETEM) at the atomic level. The in situ results reveal distinct formation behaviors of TiO2-x overlayers: complete, partial, and no encapsulation of Ni nanoparticles (NPs) on the {100}, {101}, and {001} TiO2 facets, respectively. Complementary in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), X-ray absorption spectroscopy (XAS) experiments and density functional theory (DFT) calculations further reveal a dual induction mechanism, where adsorbates both participate in TiO2-x formation and stabilize the encapsulating overlayer. Moreover, TiO2-x transfers electrons to Ni and stabilizes COOH* intermediates that dehydroxylate to form CO. Guided by these mechanistic insights, facet-dependent A-SMSI enables remarkable selectivity modulation, yielding CH4 selectivity exceeding 88% on Ni/TiO2-{001} and CO selectivity over 83% on Ni/TiO2-{100}. These findings advance the fundamental understanding of A-SMSI and offer a rational framework for designing oxide-supported catalysts with tailored interfacial properties.