Hedgehog-like Pd/Nitride Nanocone Facilitates Bubble Detachment for High-Rate Photothermal Hydrogen Release.

Abstract

The practical application of formic acid for large-scale hydrogen storage is constrained by its low H₂ production rates. Conventional strategies rely on excessive chemical additives to accelerate the initial deprotonation step for efficient dehydrogenation. However, this approach is energy-consuming and compromises the intrinsic hydrogen storage density (53 g L^-1) of formic acid. Here, we tackle this challenge by designing a floatable photothermal reaction platform featuring hedgehog-like Pd-nitride nanocones supported on carbon fiber sheets. Leveraging the structure-induced floating and superaerophobicity design, this platform enables instantaneous bubble detachment from reactive sites, facilitating local product removal and thereby propelling deprotonation without additives. Consequently, an exceptional H₂ production rate of 478 mmol g^-1 h^-1 was achieved from pure formic acid, tripling the rate of the current top-performing catalytic materials. This strategy offers fresh perspectives into liquid hydrogen carrier dehydrogenation, enabling simultaneously high-rate hydrogen production and high hydrogen storage density.