Two-Dimensional Supramolecular Nanoarchitectures of Polypseudorotaxanes Based on Cucurbit[8]uril for Highly Efficient Electrochemical Nitrogen Reduction

Supramolecular assemblies with two-dimensional (2D) topology have drawn great attraction in the development of functional materials through a modular approach. Herein, a novel organic 2D polypseudorotaxane has been constructed on the basis of cucurbit[8]uril (CB[8]) through host-stabilized charge-transfer (CT) interactions of naphthol-modified porphyrin (TPP-Np) and viologen derivatives (DMV). Interestingly, the 2D polypseudorotaxanes could serve as a platform for preparation of ultrafine Pt nanoparticles with favorable and homogeneous dispersion through a simple self-metallized process, leading to the formation of supramolecular hybrid materials (PtNPsp(CB[8]/DMV/TPP-Np)). Surprisingly, the PtNPsp(CB[8]/DMV/TPP-Np) could be applied to efficient electrochemical nitrogen reduction reaction, with a NH3 yield rate up to 23.2 mu g h(-1) mg(Pt)(-1) at -0.2 V versus a reversible hydrogen electrode under ambient conditions. Notably, our results not only demonstrate the feasible construction of 2D polypseudorotaxanes but also deepen the understanding of structure-activity relationships in supramolecular nanoarchitectures, as well as pave an effective and low-energy input strategy for artificial nitrogen fixation.