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<p>Targeting the demand for efficient dehydrogenation catalysts in liquid organic hydrogen carriers, we synthesized a series of La-doped alumina supports by a co-precipitation/hydrothermal route and deposited Pd nanoparticles to promote 12H-N-propylcarbazole (NPCZ) dehydrogenation. Comprehensive characterization shows that an optimal 10 wt % La loading generates intimately interfaced La<sub>2</sub>O<sub>3</sub> and La(OH)<sub>3</sub> nanodomains that anchor highly dispersed Pd particles (∼2.2 nm), donate electrons to Pd<sup>0</sup>, and create bifunctional acid-base sites together with a fast hydrogen-spillover network. These synergistic features accelerate C–H activation and H-migration, enabling Pd/La<sub>10</sub>AlO to deliver the theoretical H<sub>2</sub> release (5.43 wt %) in 150 min at 180 °C with 99% NPCZ selectivity and no activity loss over ten cycles. Kinetic analysis reveals markedly lower apparent activation energies for all three successive dehydrogenation steps, with a ∼65 kJ·mol<sup>−1</sup> drop in the rate-limiting 4H-NPCZ→NPCZ stage, underscoring the thermodynamic and kinetic benefits conferred by the dual-phase La promoter. This work provides the first mechanistic evidence that coexisting La<sub>2</sub>O<sub>3</sub>/La(OH)<sub>3</sub> can cooperatively tune the electronic and interfacial structure of Pd/Al<sub>2</sub>O<sub>3</sub>, offering clear guidelines for designing durable, high-performance dehydrogenation catalysts for N-heterocyclic liquid organic hydrogen carriers.</p>

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Synergistic La2O3-La(OH)3 interface engineering enables deep and durable dehydrogenation of 12H-N-propylcarbazole over Pd/Al2O3 catalysts

  • 期刊论文

  • 发表日期：

    2025年7月31日

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  • Li Liu,
  • Tian Wu,
  • Yu Zhang,
  • Chenggen Li,
  • Yuan Dong,
  • Ming Yang

摘要

Targeting the demand for efficient dehydrogenation catalysts in liquid organic hydrogen carriers, we synthesized a series of La-doped alumina supports by a co-precipitation/hydrothermal route and deposited Pd nanoparticles to promote 12H-N-propylcarbazole (NPCZ) dehydrogenation. Comprehensive characterization shows that an optimal 10 wt % La loading generates intimately interfaced La2O3 and La(OH)3 nanodomains that anchor highly dispersed Pd particles (∼2.2 nm), donate electrons to Pd0, and create bifunctional acid-base sites together with a fast hydrogen-spillover network. These synergistic features accelerate C–H activation and H-migration, enabling Pd/La10AlO to deliver the theoretical H2 release (5.43 wt %) in 150 min at 180 °C with 99% NPCZ selectivity and no activity loss over ten cycles. Kinetic analysis reveals markedly lower apparent activation energies for all three successive dehydrogenation steps, with a ∼65 kJ·mol−1 drop in the rate-limiting 4H-NPCZ→NPCZ stage, underscoring the thermodynamic and kinetic benefits conferred by the dual-phase La promoter. This work provides the first mechanistic evidence that coexisting La2O3/La(OH)3 can cooperatively tune the electronic and interfacial structure of Pd/Al2O3, offering clear guidelines for designing durable, high-performance dehydrogenation catalysts for N-heterocyclic liquid organic hydrogen carriers.