A Dynamic Self-Reporting Metal–Organic Framework System for Catalysis and Real-Time Reaction Monitoring

Abstract Modern catalysis research has primarily focused on improving catalyst activity, selectivity, and stability through active-site engineering, microenvironment regulation, and mechanistic understanding. However, the sustainability and efficiency of catalytic processes also depend on the dynamic evolution of reaction systems, including substrate consumption, catalyst deactivation, and product accumulation. Despite their importance, these changes are typically assessed by off-line analysis rather than real-time monitoring, which hinders efficient process optimization and sustainable operation. Here, we develop a dynamic self-reporting (DSR) catalytic system based on Ag@UiO-66-(COOH)2/NDCA that simultaneously functions as a heterogeneous oxidation catalyst and an optical reporter for reaction progress. During oxidation, the emission intensity at 440 nm increases with product formation and exhibits a strong quantitative correlation with benzaldehyde yield, enabling reaction progress to be continuously tracked across a series of substituted benzyl alcohols. Mechanistic studies indicate that the luminescence response is governed by competitive absorption and substrate-dependent interactions. Density functional theory calculations further reveal that benzyl alcohol forms stronger dispersion-stabilized π···π interactions with the emissive NDCA2– linkers than benzaldehyde, resulting in more pronounced luminescence quenching. As benzyl alcohol is converted into the more weakly interacting product, this quenching is progressively relieved, producing a measurable increase in emission intensity that reports the reaction progress. This integration provides a platform for reaction monitoring, process optimization, and future automated manufacturing.