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美崎 慧*; 三輪 寛子*; 伊藤 孝; 吉田 健文*; 長谷川 慎吾*; 中村 由紀奈*; 徳竹 駿太*; 高畠 萌*; 下村 浩一郎*; Chun, W.-J.*; et al.
ACS Catalysis, 13(18), p.12281 - 12287, 2023/09
被引用回数：1 パーセンタイル：46.87(Chemistry, Physical)The direct alkylation of benzenes with simple alkanes is one of the ideal processes for the production of alkylbenzenes. We demonstrated that Pd nanoparticles on the outer surface of H-ZSM-5 are efficient catalysts for direct alkylation. The reaction proceeds through the activation of an alkane on the acid sites present inside the zeolite pores. This process is followed by the nucleophilic addition of an arene to the activated alkane. The spillover of the abstracted hydrogen atoms from the acid sites to the Pd nanoparticles on the outer surface accelerates recombination to H
. A maximum toluene conversion of 58.5% and selectivity of 95.6% for the alkylated products are achieved when toluene is reacted with 
-heptane. 
-selective alkylation is achieved, due to the effect of the pore size of H-ZSM-5. The 
SR study of muonium, a pseudo-isotope of hydrogen, in aluminosilicates suggested that the formation of atomic hydrogen is possible and its lifetime is in the sub-microsecond range or longer, which is long enough for chemical reactions.
加藤 優*; 藤林 那月*; 阿部 大輝*; 松原 直啓*; 保田 諭; 八木 一三*
ACS Catalysis, 11(4), p.2356 - 2365, 2021/02
被引用回数：36 パーセンタイル：88.11(Chemistry, Physical)Fe-N-C酸素還元反応触媒は高分子電解質燃料電池のキーマテリアルである。しかしながら、多くのFe-N-C電極触媒は、副生成物としてH
Oが生成されるため、生成物の選択性に問題がある。本研究では、Cu, Fe、およびNをドープしたカーボンナノチューブのORR電極触媒を合成した。このヘテロバイメタル触媒は、OからHOへの高い選択性を有する4電子還元を示した。酸性中での酸素還元および過酸化水素還元反応の速度論的分析を行った結果、Cu, Fe-Nドープ触媒は、OからHOへの直接4電子還元の速度定数が、電子還元の速度定数よりも桁も高いことが明らかになった。一方、OからHOへの変化に対して、Fe-Nドープ触媒は同程度の大きさを示し、異種金属の協同性がORRキネティックに劇的な影響を与えたことを示す結果が得られた。
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：158 パーセンタイル：96.49(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
mol
min, 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
) and positively charged Ni (Ni
) in the Pt-Ni alloy are prone to interact with H and OH of HO molecules, respectively, leading to an energetically favorable reaction pathway.
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：18 パーセンタイル：43.96(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
Pt
O
and CaZrPtO. 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.
