Dual Zn5−NiS4 Sites in a Redox‐Active Metal–Organic Framework Enables Efficient Cascade Catalysis for Nitrate‐to‐Ammonia Conversion

-cluster-based MOFs applied for the investigation of electrocatalytic nitrate reduction. Our results indicated that substitution by -thienyl instead of -phenyl group increases the S-heteroatom content, improves the conductivity and facilitates electron transfer. Furthermore, Density Functional Theory (DFT) calculations of the energy changes for the reduction of each species could rationalize experimental results.