Improved Low‐Temperature Hydrogen Production from Aqueous Methanol Based on Synergism between Cationic Pt and Interfacial Basic LaOx

Abstract

AbstractAqueous phase reforming of methanol (APRM) is simple, inexpensive and provides a high hydrogen gravimetric density of 18.8 wt. %, and so is superior to traditional gas‐phase reactions performed at relatively high temperatures. In the present work, the interface between Pt nanoparticles and a TiN support was modified using a highly dispersed amorphous LaOx phase. The resulting Pt/LaOx/TiO(N) exhibited enhanced activity and long‐term stability during the APRM reaction under base‐free conditions compared with Pt catalysts supported on unmodified TiN or crystalline La2O3. The interfacial amorphous LaOx phase promoted the deposition of small Pt nanoparticles having a narrow size distribution, and also generated electron‐deficient Pt. An assessment of kinetic isotope data and theoretical investigations demonstrated that the cationic Pt nanoparticles facilitated the cleavage of O−H and C−H bonds in methanol while the amorphous LaOx enhanced the dissociation of water, thus enabling the water‐gas shift reaction under mild conditions.