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Electroactive Metal-Organic Frameworks as Emitters for Self-Enhanced Electrochemiluminescence in Aqueous Medium.

Metal-organic frameworks (MOFs) have limited applications in electrochemical fields due to their poor conductivity. In this work, an electroactive MOF (E-MOF) is designed as a highly crystallized electrochemiluminescence (ECL) emitter in aqueous medium for the first time. The E-MOF contains mixed-ligands of hydroquinone and phenanthroline as oxidative and reductive couples, respectively. Interestingly, E-MOFs demonstrate excellent performance with surface state model in both co-reactant and annihilation ECL in aqueous medium. Compared with the individual components, E-MOFs significantly improve the ECL emission due to the framework structure. More importantly, the self-enhanced ECL emission with high stability is realized by the accumulation of MOF's cation radicals via pre-reduction electrolysis. The self-enhanced mechanism is theoretically identified by density functional theory. The mixed-ligand E-MOFs provide a proof of concept using molecular crystalline materials as new ECL emitters for fundamental mechanism studies, and broadens their applications in long-term ECL assays.