Publication date: 15th December 2025
The use of a well-defined supramolecular cage to encapsulate a catalytic molecule in order to confer an enhancement to its activity is an attractive strategy in chemical catalysis, though functional examples in electrocatalysis are exceedingly rare.
Against this backdrop, this work investigates the microenvironment-confined catalytic activity of a Co-bearing porphyrin encapsulated within a cubic Fe8L6 cage with Zn-porphyrin faces. We show that the encapsulated Co-porphyrin exhibits approx. 10-fold enhanced electrocatalytic current densities and much higher Faradaic efficiencies for nitrate reduction to ammonia relative to the free Co-porphyrin analogue. Quantitatively, the supramolecular catalyst attains a reaction selectivity nearing 100% for NH3, a partial current density of 351 mA cm–2, a turnover frequency of 742 s–1 and a turnover number of 108 million, metrics substantially higher than those for the free Co-porphyrin.
This system is conceptually different to the use of isolated active sites and cage-like catalysts that catalyse reactions outside of the cage without beneficial microenvironment effects. In contrast, by designing a supramolecular cage with the active site solely located inside of the cage, we attained a true catalytic cavity with the microenvironment serving as an orthogonal lever to boost performance. Mechanistic investigations suggest that the activity is enhanced due to: 1) a tandem catalytic mechanism in which the NO3– → NO2– reduction is carried out preferentially on the Zn sites and the subsequent NO2– → NH3 steps occur on the Co site, and 2) a catalytic microenvironment that substantially accelerates the latter NO2– reduction steps.
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