Dual Functionality of a Plasmonic Gold Photocatalyst in the Reversible Dehydrogenation / Hydrogenation of N ‐Heterocycles

ABSTRACT LOHC (Liquid Organic Hydrogen Carrier) systems have emerged as a promising strategy for hydrogen storage and distribution. Among these, N ‐Heterocycles stand out due to their high hydrogen capacity. Their photocatalytic dehydrogenation has attracted significant attention due to the environmentally friendly conditions under which the reaction can proceed. We report here a new hybrid plasmonic material in which a covalent organic framework (COF) serves as a stabilizing matrix for gold nanoparticles, grafted in situ via an organometallic approach, with sizes ranging from 2 to 4 nm. We have employed the synthesized material as a recyclable photocatalyst in a light‐mediated dehydrogenation of N ‐Heterocycles. This new carbon‐based semiconductor photocatalyst also introduces a novel photocatalyst capable of generating both dehydrogenation and hydrogenation products by simply changing the reaction conditions, offering a significant advance for hydrogen storage.