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In this work, a single crystal catalyst was synthesized via protective desilication of zeolite while incorporating indium. Glucose was isomerized in methanol at concentrations as high as 33\u2005wt\u2009% before being hydrolyzed with water. The final fructose production was 54.9\u2009%, with 89.1\u2009% selectivity and 93.3\u2009% sugar recovery, the highest isomerization rate at the highest concentration ever reported. Indium was present in the single\u2010crystal catalyst as oxide nanoparticles and boundary framework atoms, and it achieved intelligent cooperation in the production of fructose syrup in methanol by catalyzing isomerization and selective glycosidation, minimizing degradation due to fructose accumulation and eliminating side reactions. 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