Ultralow Pd bimetallic catalysts boost (de)hydrogenation for reversible H2 storage

• Published in: Applied catalysis. B, Environmental Environmental, 2024-04, Vol.343, p.123574, Article 123574
• Main Authors: Xue, Wenjie, Zhao, Binbin, Liu, Hongxia, Chen, Xinqing, Liu, Lei
• Format: Article
• Language: English
• Subjects: (De)hydrogenation; Bimetallic catalyst; Density functional theory; Liquid organic hydrogen carrier; N-propylcarbazole
• ISSN: 0926-3373; 1873-3883
• DOI: 10.1016/j.apcatb.2023.123574

The facile catalytic reversible (de)hydrogenation of liquid organic hydrogen carriers (LOHC) using a single catalyst holds great value for onboard hydrogen storage. Herein, we develop a bimetallic catalyst Pd1Ni based on nonnoble metal Ni with ultralow Pd of 0.05 wt%, which enables reversible (de)hydrogenation of NPC and supports multiple cycles of reversible hydrogen uptake and release. Notably, the bimetallic catalyst Pd1Ni exhibits more excellent catalytic performance on the dehydrogenation reaction of dodecahydro-N-propylcarbazole (12H-NPC) than the 1%Pd catalyst and similar catalytic performance on the hydrogenation reaction of NPC compared to the 1%Ru catalyst. The astonishing catalytic efficiency of Pd1Ni catalysts is due to the ideal electronic structure between ultralow Pd and Ni NPs allowing rapid interfacial electron transfer to intermediates, as revealed by structural analyses and density functional theory (DFT) computations. [Display omitted] •Design one single Pd1Nicatalyst capable of driving both hydrogenation of NPC and dehydrogenation of dodecahydro-NPC (12H-NPC).•Pd1Nicatalyst allows multiple cycles of reversible hydrogen uptake and release.•Pd1Nicatalyst exhibits more excellent catalytic performance on the (de)hydrogenation of dodecahydro-NPC (12H-NPC) than 1%Pd and 1%Ru catalyst.•The plausible mechanism of the (de)hydrogenate of NPC on Pd1Nicatalystswereproposedby DFT calculation.