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Herein, a cluster\u2010defect engineering (CDE) strategy is employed to modify the pristine UiO\u201066 framework, wherein Zn incorporation followed by selective acid etching yields defect\u2010rich A\/(Zn,Zr)UiO\u201066 catalysts featuring hierarchical porous architectures and abundant Lewis (L) acid sites. Optical and photoelectrochemical analyses confirm that CDE broadens visible\u2010light harvesting, narrows the bandgap, and prolongs carrier lifetimes. The synergistic interplay between L acid sites and photocatalysis over A\/(Zn,Zr)UiO\u201066 results in an excellent photocatalytic performance in biodiesel production via oleic acid (OA) esterification with methanol (CH\n                    <jats:sub>3<\/jats:sub>\n                    OH) under mild reaction conditions, outperforming pristine UiO\u201066. Notably, the optimized A\/(Zn,Zr)UiO\u201066\u20100.2 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\n                    <jats:sub>3<\/jats:sub>\n                    O\u2022 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\u2010light\u2010driven biomass upgrading and sustainable fuel production.\n                  <\/jats:p>","DOI":"10.1002\/anie.5124107","type":"journal-article","created":{"date-parts":[[2026,5,14]],"date-time":"2026-05-14T09:06:58Z","timestamp":1778749618000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":12,"title":["Synergistic Lewis Acid Photocatalysis Over Cluster\u2010Defect\u2010Engineered UiO\u201066 for Efficient Liquid Biomass Upgrading"],"prefix":"10.1002","volume":"65","author":[{"given":"Hao","family":"Wang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Green Pesticide State\u2010Local Joint Laboratory For Comprehensive Utilization of Biomass Center For R&amp;D of Fine Chemicals of Guizhou University  Guiyang P. R. 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