Unlocking Enhanced Hydrogen Storage in Naphthalene via K‐Induced Acidity and Metal Dispersion in Dendritic Catalysts

ABSTRACT Novel dendritic ZSM‐22/DMSNs (ZD) micro‐mesoporous composites with center–radial pore structure and suitable acidity were developed by nano‐assembly strategy. Subsequently, Pt/ZD‐K catalysts were synthesized based on the principle of electrostatic adsorption, with the states of active phase regulated by alkali metal additives K. The incorporation of K regulated the acidity, improved the dispersion of Pt particles, and altered the electronic state of Pt species, leading to more Pt δ+ and Pt 0 species. The catalyst with a K/Pt molar ratio of 1 (Pt/ZD‐1K) presented outstanding performance of hydrogen storage in naphthalene among the Pt/ZD‐K catalysts designed, reaching 100% hydrogenation conversion of naphthalene and 100% yield of decalin. The reaction rate constant reached 5.2 × 10 −2 mol g −1 h −1 , whereas the turnover frequency value was 1464 h −1 . The exceptional hydrogenation performance of Pt/ZD‐1K is due to the synergistic effects of the excellent textural properties, abundant acidity, highly dispersed Pt particles, and a large number of Pt 0 and Pt δ+ species. Besides, the reaction mechanism of hydrogen storage in naphthalene was explored and proposed for such Pt/ZD‐K catalysts.