| 研究課題/領域番号 |
21J10648
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| 研究種目 |
特別研究員奨励費
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| 配分区分 | 補助金 |
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| 応募区分 | 国内 |
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| 審査区分 |
小区分28030:ナノ材料科学関連
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| 研究機関 | 大阪大学 |
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研究代表者 |
PHAM THANH NGOC (2021) 大阪大学, 工学研究科, 特別研究員(DC2)
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| 特別研究員 |
PHAM THANH NGOC (2022) 大阪大学, 工学研究科, 特別研究員(DC2)
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| 研究期間 (年度) |
2021-04-28 – 2023-03-31
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| 研究課題ステータス |
完了 (2022年度)
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| 配分額 *注記 |
1,500千円 (直接経費: 1,500千円)
2022年度: 700千円 (直接経費: 700千円)
2021年度: 800千円 (直接経費: 800千円)
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| キーワード | Pd / SrTiO3 / sintering / MSI / three-way catalyst / NO reduction reaction |
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| 研究開始時の研究の概要 |
In this research, we aim to elucidate and design nitric oxide (NO) reduction reaction (NORR) in the three-way catalyst (TWC) by first-principles multiscale simulation. The atomic structures of supported metal clusters shall be revealed by global optimization, and accurate potential energy diagrams for NORR will be studied by reaction path search. We expect to obtain a detailed correlation between atomic structures and their reaction activity, which may be helpful to design NORR in TWC.
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| 研究実績の概要 |
In this fiscal year, we studied the binding strength of Pd clusters supported on SrO- and TiO2- terminated SrTiO3 (SrO-STO-113 and TiO2-STO-113) perovskite to elucidate the metal support interaction (MSI) of Pd/SrTiO3 catalyst under real three-way catalyst operating condition. We systematically sampled several PdxOy clusters supported on SrO-STO-113 and TiO2-STO-113; as well as PdxOy clusters on gamma-Al2O3 (100) by using machine-learning enhanced global optimization (GOFEE) methods. Oxidation of several small Pd clusters is assessed by atomistic thermodynamics from a set of global minimums of STO-supported PdxOy. Structural properties and interfacial bonding were evaluated in detail. The square-planar PdO4 motif is found to be an elementary building block of oxidized clusters. We found that small metallic Pd clusters with an oxygen vacancy at the substrate underneath is stable under the reductive atmosphere, while PdO-like clusters are stable under stoichiometric and oxidative ones. We find that the MSI is further increased upon the oxidation of Pd clusters on both STO and gamma-Al2O3 surfaces, implying that the oxidative pretreatment will increase the thermal stability of the TWC. Moreover, compared with conventional gamma-Al2O3, MSI of small PdxOy clusters and STO (001) surfaces is much stronger driven by greater charge transfer interaction. The growth of small oxidized PdxOy clusters is also studied and some “magic” numbers in term of stability against the Otsward ripening are found. Our results indicate Pd/STO catalysts has higher thermal stability.
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| 現在までの達成度 (段落) |
令和4年度が最終年度であるため、記入しない。
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| 今後の研究の推進方策 |
令和4年度が最終年度であるため、記入しない。
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