| 研究課題/領域番号 |
19F19059
|
|---|
| 研究種目 |
特別研究員奨励費
|
| 配分区分 | 補助金 |
|---|
| 応募区分 | 外国 |
|---|
| 審査区分 |
小区分27030:触媒プロセスおよび資源化学プロセス関連
|
|---|
| 研究機関 | 北海道大学 |
|---|
研究代表者 |
清水 研一 北海道大学, 触媒科学研究所, 教授 (60324000)
|
|---|
| 研究分担者 |
LIU CHONG 北海道大学, 触媒科学研究所, 外国人特別研究員
|
|---|
| 研究期間 (年度) |
2019-04-25 – 2021-03-31
|
| 研究課題ステータス |
完了 (2020年度)
|
| 配分額 *注記 |
2,300千円 (直接経費: 2,300千円)
2020年度: 1,100千円 (直接経費: 1,100千円)
2019年度: 1,200千円 (直接経費: 1,200千円)
|
|---|
| キーワード | NH3-SCR / O2 activation / zeolites / dehydrogenation / ethane / DFT |
|---|
| 研究開始時の研究の概要 |
８．研究の概要
The direct non-oxidative conversion of methane into aromatics and hydrogen (methane dehydroaromatization, MDA) is one of the most promising processes. The research project will focus on the understanding of the fundamental factors that control the catalytic performance of MDA reaction. The reaction mechanism of MDA will be investigated using state-of-the-art computational approaches to provide molecular-level insights, aiming to deliver practical solutions for MDA optimization and to benefit on the catalyst design for efficient methane upgrading.
|
| 研究実績の概要 |
Selective catalytic reduction of nitrogen oxides using ammonia (NH3-SCR) over Cu-exchanged zeolites is an important process and proceeds via reduction of Cu(II) to Cu(I) and subsequent reoxidation of Cu(I) to Cu(II). Although the mechanism of reduction half cycle has been relatively well established, reoxidation pathways of Cu(I) to form the original Cu(II) species are highly complicated and remain unclear. In our study, oxidation mechanisms of Cu(I) to Cu(II) species in CHA zeolites during the NH3-SCR process were investigated by periodic DFT calculations. The NH3-solvated Cu(I) and Cu(II) species were considered for exploring the oxidative activation reaction pathways. The results show that, with O2 as the sole oxidant, Cu(I) can be effectively oxidized to Cu(II) via multinuclear Cu-oxo intermediates with moderate reaction barriers. The NO-assisted oxidation of Cu(I) was found to favor the formation of Cu nitrate/nitrite species, which seem to only act as off-cycle resting states. We propose that reoxidation of Cu(I) to Cu(II) with O2 as the sole oxidant plays a key role in the oxidation half cycle under standard NH3-SCR conditions. The obtained information would be important for various catalytic processes over cation-exchanged zeolites.
|
| 現在までの達成度 (段落) |
令和2年度が最終年度であるため、記入しない。
|
| 今後の研究の推進方策 |
令和2年度が最終年度であるため、記入しない。
|
