Hydrogen is a promising candidate to replace the exhausting fossil fuels. However, it is still a big challenge for hydrogen storage. Liquid organic hydrogen carrier (LOHC), which possesses high safety and purity, easy transport and reversibility, is highly attractive for hydrogen storage. Herein we report a new reusable bimetallic Pd-Rh nanoparticles (NPs) catalyst with synergy effect, boosting both the hydrogenation of N-ethylcarbazole (NEC) and dehydrogenation of dodecahydro-N-ethylcarbazole (12H-NEC), which allows multiple cycles of reversible high-weight% hydrogen storage and uptake in short reaction time. Various ex- and in-situ characterizations evidenced that the superior activity was attributed to the bimetallic Pd-Rh NPs cluster structure on the surface of γ-Al₂O₃ support. The mechanism of NEC hydrogenation over the Pd-Rh catalyst was proposed and verified by density functional theory (DFT) calculations. Such a strategy can be extended to other LOHCs and sheds light onto the development of LOHCs as energy vectors.

氢是替代排放化石燃料的有前途的候选人。然而，对于储氢仍然是一个巨大的挑战。具有高安全性和纯度，易于运输和可逆性的液态有机氢载体（LOHC）在储氢方面极具吸引力。在本文中，我们报告了一种具有协同效应的新型可重复使用的双金属Pd-Rh纳米粒子（NPs）催化剂，既促进了N-乙基咔唑（NEC）的氢化作用，又促进了十二氢-N-乙基咔唑（12H-NEC）的脱氢作用，从而实现了多个可逆循环高重量％的氢存储和在短的反应时间内被吸收。各种EX-和原位表征证明了优良的活性归因于表面上，双金属钯-铑的NP簇结构的γ-Al ₂ ö ₃支持。提出了NEC在Pd-Rh催化剂上加氢的机理，并通过密度泛函理论（DFT）计算进行了验证。这样的策略可以扩展到其他LOHC，并为LOHC的发展提供了能量载体。