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論文

Atomically dispersed Pt on the surface of Ni particles; Synthesis and catalytic function in hydrogen generation from aqueous ammonia-borane

Li, Z.*; He, T.*; 松村 大樹; Miao, S.*; Wu, A.*; Liu, L.*; Wu, G.*; Chen, P.*

ACS Catalysis, 7(10), p.6762 - 6769, 2017/10

 被引用回数:102 パーセンタイル:96.66(Chemistry, Physical)

We report herein that the single-atom alloy (SAA) made of atomically dispersed Pt on the surface of Ni particles (Pt is surrounded by Ni atoms) exhibits improved catalytic activity on the hydrolytic dehydrogenation of ammonia-borane, a promising hydrogen storage method for onboard applications. Specifically, an addition of 160 ppm of Pt leads to ca. 3-fold activity improvement in comparison to that of pristine Ni/CNT catalyst. The turnover frequency based on the isolated Pt is 12000 mol$$_{rm{H}2}$$ mol$$_{rm{Pt}}$$$$^{-1}$$ min$$^{-1}$$, which is about 21 times the value of the best Pt-based catalyst ever reported. Our simulation results indicate that the high activity achieved stems from the synergistic effect between Pt and Ni, where the negatively charged Pt (Pt$$^{delta -}$$) and positively charged Ni (Ni$$^{delta +}$$) in the Pt-Ni alloy are prone to interact with H and OH of H$$_{2}$$O molecules, respectively, leading to an energetically favorable reaction pathway.

論文

Towards optimizing the performance of self-regenerating Pt-based perovskite catalysts

Jarrige, I.*; 石井 賢司; 松村 大樹; 西畑 保雄; 吉田 雅洋*; 岸 浩史*; 谷口 昌司*; 上西 真里*; 田中 裕久*; 笠井 秀明*; et al.

ACS Catalysis, 5(2), p.1112 - 1118, 2015/02

 被引用回数:14 パーセンタイル:43.47(Chemistry, Physical)

Self-regenerating automotive catalysts owe their remarkable performance to the repeated motion of the precious metal atoms in and out of the perovskite lattice under fluctuating oxidizing and reducing conditions, preventing coalescence of the metal nanoparticles. Here we use resonant inelastic X-ray scattering to characterize the occupied and unoccupied Pt 5d states in two self-regenerating Pt-perovskite catalysts, CaTi$$_{0.95}$$Pt$$_{0.05}$$O$$_3$$ and CaZr$$_{0.95}$$Pt$$_{0.05}$$O$$_3$$. Upon reduction, the element and symmetry-specific charge excitation spectra reveal a sizeable hybridization between the Pt 5d and the Ti 3d or Zr 4d states at the interface between the nanoparticles and the perovskite, which involves the occupied states and is thus invisible in X-ray absorption spectra. A correlation is found between the strength of this d-band hybridization and the proportion of Pt nanoparticles that remain buried below the surface during reduction, indicating that the motion of the Pt atoms towards the surface is hindered by this hybridization specifically, rather than by the Pt-O bonding. These results provide direct evidence that the strength of the metal-metal d-band hybridization plays a pivotal role in determining the efficiency of self-regeneration in perovskite catalysts.

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