Mixed-valence Ru nanoparticles anchored on N-rich metal-phthalocyanine/graphene vdW heterostructures for
Zichong Xiang1, Guanping Wei1, Aifeng Yang1
1College of Chemistry and Materials, Gannan Normal University Ganzhou 341000 China longbin-li@gnnu.edu.cn ywchen@gnnu.edu.cn.
Abstract:
Hydrogen production via alkaline anion-exchange membrane H2O electrolysis (AEMWE) is constrained by sluggish hydrogen evolution reaction (HER) kinetics associated with H2O dissociation and hydroxyl management. Here, we report a pyrolysis-free Ru nanoparticles anchored on a two-dimensional metal-phthalocyanine/graphene vdW heterostructure (Ru@NiFe PPc) electrocatalyst for alkaline HER. The N-rich macrocyclic phthalocyanine framework and strong Ru-N coordination enable the uniform and stable dispersion of the mixed-valence Ru nanoparticles. The high-valence Ru centers accelerate interfacial H2O dissociation and hydroxyl transfer, whereas the Ru0 sites facilitate *H desorption. Thus, Ru@NiFe PPc delivers exceptional HER performance with only 15 mV at 10 mA cm-2, surpassing the best-performing Ru-based catalysts. As an AEMWE cathode, Ru@NiFe PPc delivers an industrial-scale current density of 2.0 A cm-2 at 2.09 V. In a hybrid electrolyzer coupling HER with low-potential 5-hydroxymethylfurfural oxidation, the system delivers 100 mA cm-2 at an ultralow cell voltage of 0.30 V. Theory calculations reveal that hydrogen-bond-assisted H2O adsorption on Ru nanoparticles, and the electronic coupling between Ru nanoparticles and phthalocyanine matrix weakens *OH binding, effectively lowering the overall HER barrier. This work elucidates the full alkaline HER pathway involving all key intermediates and opens a new avenue for the design of pyrolysis-free Ru-based HER catalysts.
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