Synergistic Lewis Acid Photocatalysis Over Cluster‐Defect‐Engineered UiO‐66 for Efficient Liquid Biomass Upgrading
4 affiliations
- 1State Key Laboratory of Green Pesticide State‐Local Joint Laboratory For Comprehensive Utilization of Biomass Center For R&D of Fine Chemicals of Guizhou University Guiyang P. R. China
- 2ARC Industrial Transformation Research Hub for Intelligent Energy Efficiency in Future Protected Cropping (E2Crop) Melbourne VIC Australia
- 3Centre For Atomaterials and Nanomanufacturing (CAN) School of Science RMIT University Melbourne Australia
- 4College of Materials and Chemical Engineering Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials China Three Gorges University Yichang P. R. China
Abstract
Defect engineering provides new opportunities to overcome the intrinsic limitations of metal–organic frameworks (MOFs) in photocatalysis. Herein, a cluster‐defect engineering (CDE) strategy is employed to modify the pristine UiO‐66 framework, wherein Zn incorporation followed by selective acid etching yields defect‐rich A/(Zn,Zr)UiO‐66 catalysts featuring hierarchical porous architectures and abundant Lewis (L) acid sites. Optical and photoelectrochemical analyses confirm that CDE broadens visible‐light harvesting, narrows the bandgap, and prolongs carrier lifetimes. The synergistic interplay between L acid sites and photocatalysis over A/(Zn,Zr)UiO‐66 results in an excellent photocatalytic performance in biodiesel production via oleic acid (OA) esterification with methanol (CH 3 OH) under mild reaction conditions, outperforming pristine UiO‐66. Notably, the optimized A/(Zn,Zr)UiO‐66‐0.2 achieves a remarkable 99.3% biodiesel yield under mild conditions, alongside superior stability and reusability. Further, in situ spectroscopic investigations and density functional theory (DFT) calculations disclose that CDE lowers the coupling barrier of OA and CH 3 O• radicals by strengthening OA adsorption and activation as well as facilitating charge stabilization at unsaturated Zr sites. This work highlights CDE as an ingenious strategy for tailoring the electronic configuration and interfacial chemistry of MOFs, offering a versatile platform for visible‐light‐driven biomass upgrading and sustainable fuel production.
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BibTeX
@article{wang2026synergistic,
title = {{Synergistic Lewis Acid Photocatalysis Over Cluster‐Defect‐Engineered UiO‐66 for Efficient Liquid Biomass Upgrading}},
author = {Hao Wang and Li‐Long Zhang and Haimei Xu and Baohua Jia and Liqun Ye and Tianyi Ma and Heng Zhang},
journal = {Angewandte Chemie International Edition},
year = {2026},
month = may,
doi = {10.1002/anie.5124107},
url = {https://doi.org/10.1002/anie.5124107},
note = {CC BY-NC},
}
RIS
TY - JOUR
TI - Synergistic Lewis Acid Photocatalysis Over Cluster‐Defect‐Engineered UiO‐66 for Efficient Liquid Biomass Upgrading
AU - Hao Wang
AU - Li‐Long Zhang
AU - Haimei Xu
AU - Baohua Jia
AU - Liqun Ye
AU - Tianyi Ma
AU - Heng Zhang
PY - 2026
DA - 2026/05/14
JO - Angewandte Chemie International Edition
DO - 10.1002/anie.5124107
UR - https://doi.org/10.1002/anie.5124107
AB - Defect engineering provides new opportunities to overcome the intrinsic limitations of metal–organic frameworks (MOFs) in photocatalysis. Herein, a cluster‐defect engineering (CDE) strategy is employed to modify the pristine UiO‐66 framework, wherein Zn incorporation followed by selective acid etching yields defect‐rich A/(Zn,Zr)UiO‐66 catalysts featuring hierarchical porous architectures and abundant Lewis (L) acid sites. Optical and photoelectrochemical analyses confirm that CDE broadens visible‐light harvesting, narrows the bandgap, and prolongs carrier lifetimes. The synergistic interplay between L acid sites and photocatalysis over A/(Zn,Zr)UiO‐66 results in an excellent photocatalytic performance in biodiesel production via oleic acid (OA) esterification with methanol (CH 3 OH) under mild reaction conditions, outperforming pristine UiO‐66. Notably, the optimized A/(Zn,Zr)UiO‐66‐0.2 achieves a remarkable 99.3% biodiesel yield under mild conditions, alongside superior stability and reusability. Further, in situ spectroscopic investigations and density functional theory (DFT) calculations disclose that CDE lowers the coupling barrier of OA and CH 3 O• radicals by strengthening OA adsorption and activation as well as facilitating charge stabilization at unsaturated Zr sites. This work highlights CDE as an ingenious strategy for tailoring the electronic configuration and interfacial chemistry of MOFs, offering a versatile platform for visible‐light‐driven biomass upgrading and sustainable fuel production.
SN - 1433-7851
SN - 1521-3773
ER -