Strong metal-support interactions between Pt and CeO2 for efficient methanol decomposition

Methanol decomposition is one of the most favorable chemical processes to alleviate the limitation of hydrogen storge and transportation. However, the different requirements of metal active sites for the activation of C-H and O-H bonds as well as strong adsorption of *CO intermediates limit the qualitative improvement of H2 generation for methanol decomposition. Herein, the Pt nanoparticles supported on nanorods of CeO2 with abundant oxygen defects (Pt/NR-CeO2-PD), prepared by photo-assisted deposition method, significantly boosted the H2 generation from methanol decomposition with an extremely high turnover frequency (TOF) of 84,225 h- 1 and a large turnover number (TON) of 15,020,776 (200 h) at 300 degrees C. Mechanism investigations suggested that such superior catalytic performance was derived from the strong metal-support interaction of Pt/NR-CeO2-PD, in which the abundant oxygen defect of NR-CeO2 and high electronic density of Pt contributed to the efficient activation of O-H and C-H bonds, respectively. In addition, the down-shifting of d-band center of Pt further promoted the desorption of *CO intermediates. These findings may guide the design of new catalytic systems via construction of active sites for methanol decomposition.

Automated summary

In this study, Pt nanoparticles supported on oxygen-deficient CeO2 nanorods were prepared and showed enhanced efficiency in hydrogen production from methanol decomposition. Mechanistic investigations revealed that the oxygen defects and high electronic density promoted the activation of O-H and C-H bonds, while the down-shifting of Pt's d-band center facilitated the desorption of *CO intermediates.