Xin Kang,Dongxu Wang,Jiancong Liu,Chungui Tian,He Xu,Jialu Xu,Honggang Fu
Improving the intrinsic catalytic activity of the active phases and mass transfer of the reactants and products are key issues in heterogeneous catalysis. Herein, we construct hollow zeolites with a thin shell of about 10 nm and mesopore structure as supports to load NiMoSX catalysts. On one hand, the nanocages with hollow structures can effectively confine the growth of NiMoSX catalysts, leading to a shorter slab length, higher sulfidation degree, more Ni–Mo–S active sites, and enhanced intrinsic activity. The deep hydrodesulfurization (HDS) activity for dibenzothiophene (DBT) of the NiMoSX/Hol-ZSM-5 catalyst is superior to that of NiMoSX on nanosized ZSM-5 with a reaction rate constant kHDS value of 18.74 × 10−7 mol g−1 s−1. On the other hand, the accessible nanocages and mesopore structure greatly facilitate the mass transfer process and inhibit the formation of carbon deposits, which enhances the HDS stability of NiMoSX/Hol-ZSM-5 to over 80 h. This hollow structure-confined strategy sheds light on the design of novel highly efficient supported catalysts, which we believe could be extended to other heterogeneous catalysis systems.
Alkaline water electrolysis (AWE) shows great potential for sustainable hydrogen production, but its deployment is hindered by insufficient charge/mass transfer at electrode–electrolyte interfaces. Herein, we report a distinctive heterostructure featuring NiOOH nanosheets with Ru doping immobilized on NiMoSx (RuNiOOH/NiMoSx) to address this challenge. Theoretical predictions and experimental results demonstrate that the charge redistribution in the RuNiOOH/NiMoSx heterostructure downshifts the Ru d-band center, thereby optimizing H* binding strength and the unique heterostructure provides a multitude of accessible active sites and three-dimensional (3D) mass transport channels, synergistically facilitating H2O adsorption and bubble desorption. Such optimized bubble dynamics ensure rapid active-site regeneration and sustained catalytic activity. As a consequence, the RuNiOOH/NiMoSx electrode exhibits outstanding hydrogen evolution reaction (HER) performance, delivering current densities of 10 and 500 mA cm–2 at overpotentials of 5.4 and 136.2 mV, respectively, while maintaining outstanding stability over 100 h at 100 mA cm–2. Furthermore, RuNiOOH/NiMoSx-based practical alkaline water electrolyzer drives 1.0 A cm–2 at a cell voltage of just 1.75 V for over 24 h without degradation. The present research delivers a new design paradigm for advanced heterostructured catalysts.
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