Success in making Zn+ from atomic Zn0 encapsulated in an MFI-Type zeolite with UV light irradiation

Akira Oda, Hiroe Torigoe, Atsushi Itadani, Takahiro Ohkubo, Takashi Yumura, Hisayoshi Kobayashi, Yasushige Kuroda

研究成果査読

28 被引用数 (Scopus)

抄録

For the first time, the paramagnetic Zn+ species was prepared successfully by the excitation with ultraviolet light in the region ascribed to the absorption band resulting from the 4s-4p transition of an atomic Zn 0 species encapsulated in an MFI-type zeolite. The formed species gives a specific electron spin resonance band at g = 1.998 and also peculiar absorption bands around 38,000 and 32,500 cm-1 which originate from 4s-4p transitions due to the Zn+ species with paramagnetic nature that is formed in MFI. The transformation process (Zn0 → Zn +) was explained by considering the mechanism via the excited triplet state (3P) caused by the intersystem crossing from the excited singlet state (1P) produced through the excitation of the 4s-4p transition of an atomic Zn0 species grafted in MFI by UV light. The transformation process was well reproduced with the aid of a density functional theory calculation. The thus-formed Zn+ species which has the doublet spin state exhibits characteristic reaction nature at room temperature for an O2 molecule having a triplet spin state in the ground state, forming an η1 type of Zn2+-O2- species. These features clearly indicate the peculiar reactivity of Zn+ in MFI, whereas Zn0-(H+)2MFI hardly reacts with O2 at room temperature. The bonding nature of [Zn2+-O 2-] species was also evidenced by ESR measurements and was also discussed on the basis of the results obtained through DFT calculations.

本文言語English
ページ(範囲)18481-18489
ページ数9
ジャーナルJournal of the American Chemical Society
135
49
DOI
出版ステータスPublished - 12月 11 2013

ASJC Scopus subject areas

  • 触媒
  • 化学一般
  • 生化学
  • コロイド化学および表面化学

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