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論文

Pd nanoparticles on the outer surface of microporous aluminosilicates for the direct alkylation of benzenes using alkanes

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

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$$_2$$. A maximum toluene conversion of 58.5% and selectivity of 95.6% for the alkylated products are achieved when toluene is reacted with $$n$$-heptane. ${it Para}$-selective alkylation is achieved, due to the effect of the pore size of H-ZSM-5. The $$mu^+$$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.

論文

Effects of mesopore internal surfaces on the structure of immobilized Pd-bisphosphine complexes analyzed by variable-temperature XAFS and their catalytic performances

本倉 健*; 福田 拓磨*; 上村 洋平*; 松村 大樹; 池田 まりか*; 南保 雅之*; Chun, W.-J.*

Catalysts, 8(3), p.106_1 - 106_8, 2018/03

 被引用回数:4 パーセンタイル:10.16(Chemistry, Physical)

In this study, mesoporous and nonporous silica-supported Pd complexes were synthesized and characterized. Variable-temperature XAFS measurements and a curve-fitting analysis showed a slightly larger contribution of $$sigma^{2}_{rm static}$$ when the Pd complexes were on a nonporous support in comparison to a mesoporous support. In contrast, the catalytic performance of the attached Pd complex in the Suzuki-Miyaura cross-coupling reaction was not affected by such small differences in the static disorder of the Pd complex.

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