Aqueous 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 LaO phase. The resulting Pt/LaO /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 La O . The interfacial amorphous LaO 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 LaO enhanced the dissociation of water, thus enabling the water-gas shift reaction under mild conditions.

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http://dx.doi.org/10.1002/cssc.202300283DOI Listing

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