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

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

doi:10.1007/s12209-025-00447-z

Transactions of Tianjin University ›› 2025, Vol. 31 ›› Issue (4) :421 -435. DOI: 10.1007/s12209-025-00447-z

Research Article

research-article

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

Yanyan Song ¹^,²
, Zhichao Sun ¹^,²
, Jiamin Sun ³
, Ying-Ya Liu ¹^,²^,^a
, Anjie Wang ¹^,²
, Chong Peng ¹^,²^,^b

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¹State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, 116024, Dalian, China

²Liaoning Key Laboratory of Petrochemical Technology and Equipment, Dalian University of Technology, 116024, Dalian, China

³Department of Chemistry, Division of Molecular Imaging and Photonics, KU Leuven, 3001, Louvain, Belgium

^a yingya.liu@dlut.edu.cn

^b pengchong@dlut.edu.cn

Yanyan Song

Yanyan Song pursued her master's degree in catalytic chemical engineering at the College of Chemical Engineering of Dalian University of Technology. Her research focuses mainly on the synthesis of metal-organic framework (MOF)-based photocatalytic materials and their application in the photocatalytic oxidation of benzyl alcohol to produce benzaldehyde.

Zhichao Sun

Zhichao Sun is an Associate Professor in Department of Catalysis, Dalian University of Technology (DUT). He is now investigating strategies aiming at the fields of selective hydrogenation of metals and metal phosphides, oil quality improvement, as well as catalytic reaction engineering.

Jiamin Sun

Jiamin Sun obtained her Master’s degree at Dalian University of Technology, where she focused on designing metal–organic frameworks (MOFs) for oxidative desulfurization. She then moved to Ghent University, Belgium, where she earned her PhD in Chemistry in 2023, working on the design of MOFs and covalent organic frameworks (COFs) for thermocatalysis and photocatalysis. She is currently a postdoctoral researcher at KU Leuven, Belgium. Her research interests center on the on-surface synthesis of COFs for electrocatalysis.

Ying-Ya Liu

Ying-Ya Liu is a Associate professor and Doctoral Supervisor in School of Chemical Engineering, Dalian University of Technology. Her current research interests include synthesis and applications of metal–organic frameworks, heterogeneous hydroformylation, and valorization of biomass platform compounds.

Anjie Wang

Anjie Wang is a full professor in Department of Catalysis, Dalian University of Technology (DUT). He received his Ph.D. degree from DUT in 1992. Since then, he has been teaching courses and conducting research in DUT. His research interests include synthesis of porous materials, hydrotreating catalysis, biomass conversion, non-precious metal catalysts for selective hydrogenation, plasma-aided catalysis, and catalytic reaction engineering.

Chong Peng

Chong Peng is a full professor and Doctoral Supervisor at Dalian University of Technology, Dean of the School of Chemical Engineering, Ocean Science and Life Technology, and Assistant Director of the State Key Laboratory of Fine Chemicals. A recipient of the National Science Fund for Excellent Young Scholars. His main research focuses on hydrogenation catalysts (materials) and integrated processes, as well as heterogeneous separation. He has led over 20 research projects, published over 70 SCI papers (as first & corresponding author), and holds over 200 invention patents. His work has been recognized with numerous awards, including the First Prize of Scientific and Technological Progress from the China Petroleum and Chemical Industry Federation and the Second Prize of the National Technology Invention Award.

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Abstract

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.

Keywords

Visible-light photocatalysis / Benzyl alcohol oxidation / Oxygen vacancy / Heterostructure / UiO-66-NH₂

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Yanyan Song, Zhichao Sun, Jiamin Sun, Ying-Ya Liu, Anjie Wang, Chong Peng. MOF-Derived Oxygen-Vacancy-Rich ZrO₂/UiO-66-NH₂ for Efficient Visible-Light-Driven Oxidation of Benzyl Alcohol. Transactions of Tianjin University, 2025, 31 (4) : 421-435 DOI:10.1007/s12209-025-00447-z

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