Active creation of metal-oxyl species as the reaction intermediate in partial methane oxidation by applying the reaction field of zeolite

2022 Fiscal Year Final Research Report

• Project/Area Number: 20K15297
• Research Category: Grant-in-Aid for Early-Career Scientists
• Allocation Type: Multi-year Fund
• Review Section: Basic Section 34010:Inorganic/coordination chemistry-related
• Research Institution: Nagoya University
• Principal Investigator: Oda Akira 名古屋大学, 工学研究科, 助教 (80762377)
• Project Period (FY): 2020-04-01 – 2023-03-31
• Keywords: ゼオライト / オキシル / 選択酸化触媒 / in situ分光 / 量子化学計算

Outline of Final Research Achievements

We succeeded in creating novel oxyl compounds of Ga(III) and In(III), characterizing novel ozonide compounds of Cd(II), Ga(III), and In(III), and evaluating the reactivity of Zn(II) and Ga(III) oxyl compounds. In the process of expanding our research to other metals, it became clear that the application of the oxyl creation method was limited, and we were not able to build a library on the structure/electronic state/reactivity of the oxyl compounds as much as we had originally planned. However, in the course of the study, we succeeded in designing a reaction field with the record activity for the selective oxidation of methane to formic acid, acetic acid, and methanol, respectively, and obtained new guidelines for the next phase of catalytic design studies for methane selective oxidation.

Free Research Field

無機化学、触媒

Academic Significance and Societal Importance of the Research Achievements

様々な酸化反応において金属オキシルが重要中間体として提案されているオキシルの化学はその合成難によって欠落していた。本研究では、「ゼオライト局所構造: Alサイト」の利用によりオキシルを種々の金属イオン上に安定に創製できることを示した。オキシルの状態解析、反応性評価を達成でき、新奇物性、構造や電子状態が明らかになった。ゼオライトは優れた分子ふるい能や分子集約効果及び高い熱安定性を有するため触媒や吸着材として有用性が高い。そのゼオライト細孔内にオキシルを活性点として利用することで革新的メタン転換プロセスの創成が期待される.