Now, Ding Ma, Wu Zhou and co-workers have constructed a highly stable immobilized Pt/γ-Mo₂N catalyst with a rare-earth La oxide nano-overlay for APRM, which exhibits outstanding hydrogen production activity with an exceptional turnover number (TON) of 15,300,000 \({{\rm{mol}}}_{{{\rm{H}}}_{2}}\) molmetal–1 and apparent turnover frequency (ATOF) of 24,500 \({{\rm{mol}}}_{{{\rm{H}}}_{2}}\) molmetal–1 h–1 with 0.26 wt% Pt loading and 5 wt% La loading. Impressively, 1Pt/2La-Mo2N with 1 wt% Pt loading and 2 wt% La loading maintains a high TON of 10,280,000 \({{\rm{mol}}}_{{{\rm{H}}}_{2}}\) molmetal–1 and an ATOF of 7,000 \({{\rm{mol}}}_{{{\rm{H}}}_{2}}\) molmetal–1 h–1 during 1,300 h of continuous operation. Furthermore, the hydrogen production activity of 1Pt/2La-Mo2N decreased from the peak activity by only 25%, after which it remained relatively stable for at least 100 h, indicating promising potential for a long lifespan.
A series of experiments, advanced characterization techniques and transient kinetic analysis results revealed that the inert La nano-overlay effectively protects the redundant surface sites of γ-Mo₂N from surface oxidation during APRM. Additionally, it divides the surface into partitions to confine Pt and hinder aggregation. More importantly, the universality of the inert La nano-overlay could be extended to other rare-earth elements (Y, La, Pr and Ho) as well as non-rare-earth elements (Ca, Sr and Cs). Overall, this interfacial engineering approach achieves high-activity interfacial catalysts with ultralong stability and low noble metal loading, showcasing promising potential for practical applications, especially for achieving a closed-loop hydrogen economy.
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