| 研究課題/領域番号 |
22K04821
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| 研究種目 |
基盤研究(C)
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| 配分区分 | 基金 |
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| 応募区分 | 一般 |
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| 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
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| 研究機関 | 北海道大学 |
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研究代表者 |
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| 研究期間 (年度) |
2022-04-01 – 2025-03-31
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| 研究課題ステータス |
交付 (2023年度)
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| 配分額 *注記 |
4,030千円 (直接経費: 3,100千円、間接経費: 930千円)
2024年度: 1,040千円 (直接経費: 800千円、間接経費: 240千円)
2023年度: 1,300千円 (直接経費: 1,000千円、間接経費: 300千円)
2022年度: 1,690千円 (直接経費: 1,300千円、間接経費: 390千円)
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| キーワード | Carbon Dioxde / Hydrogenation / methanol / Carbon dioxide / hydrogenation / mixed oxide catalyst / CO2 hydrogenation / Methanol / Oxide catalyst |
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| 研究開始時の研究の概要 |
Direct hydrogenation of carbon dioxide to methanol is highly attractive to reduce the use of fossil derived fuels and chemicals. However selective synthesis of methanol is challenging due to simultaneous formation of carbon monoxide. This study aims to develop multi component mixed oxide catalysts for methanol synthesis. Catalysts with oxygen vacancies will be synthesized by doping metals into metal oxide supports. Surface properties of mixed oxide will be tuned to favor the methanol formation.
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| 研究実績の概要 |
The objective of this research is to develop mixed oxide catalysts for direct hydrogenation of carbon dioxide to methanol. We previously reported that doped Co-ZrO2 catalysts were effective for stabilization of formate species and found that inclusion of In to obtain a dual atom In-Co-ZrO2 catalyst enhances methanol selectivity. In the Co-In-ZrO2 catalyst both Co and In were atomically dispersed and in close proximity of each other. Over the Co-In-ZrO2 catalyst high methanol selectivity was maintained even under low hydrogen partial pressure. Kinetic analysis of the reaction in presence of Co-In-ZrO2 showed that the presence of a dual-atom system influences the order of the reaction. Mechanistic analysis showed that the preferential adsorption of CO2 on Co sites reduces the poisoning effect of adsorbed intermediates because the In site is free for H2 dissociation. As a result, methanol selectivity as high as 86% was obtained.
Furthermore, this concept was expanded to other elements. Inclusion of Ga, Zn, also enhance the methanol selectivity and productivity. In these catalysts as well, the role of CO2 adsorption was limited to Co-Zr interface and the Ga and Zn supported H2 dissociation.
These results were summarized and published in JACS Au journal.
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| 現在までの達成度 (区分) |
現在までの達成度 (区分)
1: 当初の計画以上に進展している
理由
As per the research plan the target of FY2023 was to study the incorporation of third element to achieve high methanol selectivity and investigate the stability of the catalyst. These targets have already been achieved. The plan for FY2024 was to examine the role of each element towards the CO2 hydrogenation pathway. The mechanistic understanding of CO2 hydrogenation over the mixed oxide catalyst is already clear and it is understood that the incorporation of dual atoms alleviates the poisoning effect of adsorbed species and increases methanol selectivity. Furthermore, we have also identified additional elements that can be used in this strategy to achieve higher methanol selectivity.
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| 今後の研究の推進方策 |
The next step is to optimize the metal loading of catalyst to achieve methanol yield above the benchmark of doped metal catalysts that have been reported. Furthermore, we also target the synthesis of methanol under H2 lean conditions to maximize the use of green H2 for methanol synthesis.
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