Superaerophobic Resin‐Grafted rGO Aerogel with Boosted Product Removal Delivering High‐Performance Hydrogen Release at Ultrahigh Storage Density

Abstract Liquid hydrogen carriers featuring high hydrogen content, safety, and hydrogen release on demand have motivated great endeavors for sustainable hydrogen supply. Nonetheless, direct hydrogen release is limited by the ultralow hydrogen evolution rate, while the conventional manner of extra additive and solvent addition for promoting rates greatly deteriorates its hydrogen storage density. Thus, it is still challenging to simultaneously satisfy high‐performance hydrogen release and high storage density. Herein, an aerophobicity surface‐based gas–liquid interface reaction strategy is proposed, which renders rapid product removal to promote dehydrogenation, fundamentally circumventing the employment of additives and solvents. Accordingly, a hierarchically porous resin‐grafted reduced graphene oxide aerogel is designed. It imparts superaerophobic surface to facilitate product detachment from reactive sites, and the structure‐oriented interface reaction design provides product diffusion channels and reduced diffusion resistance. As a result, the aerogel harvests a record hydrogen evolution rate (347 mmol g −1 h −1 ) in an ultrahigh‐density formic acid of 19.8 g L −1 , around two times the rate promotion and ten times the density improvement compared to the state‐of‐the‐art materials and systems. The strategy presents an approach for the dehydrogenation of liquid hydrogen carriers, e.g., formic acid, formaldehyde, and hydrazine hydrate, concurrently ensuring high‐performance hydrogen release and high hydrogen storage density.