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<p>The development of efficient photocatalysts for selective organic transformations under visible light remains a major challenge in sustainable chemistry. In this study, we present a straightforward solvothermal strategy for fabricating a defect-engineered ZrO<sub>2</sub>/UiO-66-NH<sub>2</sub> hybrid material with abundant oxygen vacancies, enabling the visible-light-driven oxidation of benzyl alcohol to benzaldehyde. By optimizing the solvothermal treatment duration, the composite (UiO-66-NH<sub>2</sub>-2&#xa0;h) achieves a 74.1% conversion of benzyl alcohol with &gt; 99% selectivity toward benzaldehyde under mild conditions, substantially outperforming pristine UiO-66-NH<sub>2</sub>. Structural and mechanistic studies reveal that the solvothermal process induces the in situ formation of ultrasmall, uniformly dispersed ZrO<sub>2</sub> nanoparticles (~ 2.3&#xa0;nm) within the MOF matrix, while simultaneously generating abundant oxygen vacancies, as confirmed by XPS, EPR, and HRTEM analyses. The defect-mediated electronic structure of the ZrO<sub>2</sub>/UiO-66-NH<sub>2</sub> hybrid enhances visible-light absorption, facilitates charge carrier separation, and promotes efficient activation of O<sub>2</sub> into superoxide radicals (·O<sub>2</sub><sup>−</sup>), the primary reactive species. Transient photocurrent measurements and electrochemical impedance spectroscopy further verify the improved charge separation efficiency. The synergistic interplay between oxygen vacancies and the intimate ZrO<sub>2</sub>/UiO-66-NH<sub>2</sub> interface provides a unique defect-mediated charge transfer pathway, distinguishing this system from conventional heterojunctions. This study demonstrates a facile, one-step approach to integrate defect engineering with interfacial hybridization in MOF-based photocatalysts, offering a scalable route for solar-driven organic synthesis.</p> Graphical Abstract <p></p>

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MOF-Derived Oxygen-Vacancy-Rich ZrO2/UiO-66-NH2 for Efficient Visible-Light-Driven Oxidation of Benzyl Alcohol

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年8月1日

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  • Yanyan Song,
  • Zhichao Sun,
  • Jiamin Sun,
  • Ying-Ya Liu,
  • Anjie Wang,
  • Chong Peng

摘要

The development of efficient photocatalysts for selective organic transformations under visible light remains a major challenge in sustainable chemistry. In this study, we present a straightforward solvothermal strategy for fabricating a defect-engineered ZrO2/UiO-66-NH2 hybrid material with abundant oxygen vacancies, enabling the visible-light-driven oxidation of benzyl alcohol to benzaldehyde. By optimizing the solvothermal treatment duration, the composite (UiO-66-NH2-2 h) achieves a 74.1% conversion of benzyl alcohol with > 99% selectivity toward benzaldehyde under mild conditions, substantially outperforming pristine UiO-66-NH2. Structural and mechanistic studies reveal that the solvothermal process induces the in situ formation of ultrasmall, uniformly dispersed ZrO2 nanoparticles (~ 2.3 nm) within the MOF matrix, while simultaneously generating abundant oxygen vacancies, as confirmed by XPS, EPR, and HRTEM analyses. The defect-mediated electronic structure of the ZrO2/UiO-66-NH2 hybrid enhances visible-light absorption, facilitates charge carrier separation, and promotes efficient activation of O2 into superoxide radicals (·O2−), the primary reactive species. Transient photocurrent measurements and electrochemical impedance spectroscopy further verify the improved charge separation efficiency. The synergistic interplay between oxygen vacancies and the intimate ZrO2/UiO-66-NH2 interface provides a unique defect-mediated charge transfer pathway, distinguishing this system from conventional heterojunctions. This study demonstrates a facile, one-step approach to integrate defect engineering with interfacial hybridization in MOF-based photocatalysts, offering a scalable route for solar-driven organic synthesis.

Graphical Abstract