研究実績の概要 |
At the current stage, we have successfully developed pH-dependent microkinetic models for metal-nitrogen-carbon (M-N-C) catalysts for oxygen reduction reaction (ORR), in good agreement with typical experiments from literature. To further verify the models, we performed precise synthesis of molecular M-N-C catalysts and tested their ORR performance at different pH, showing excellent agreement with our models in terms of various key electrocatalytic indicators. These results show the success of this proposed research, and the main parts of the Research Plan were successfully completed. Besides, based on the grant, we extended our research to the electrochemistry-induced surface coverage effects on M-N-Cs and the structure-performance relationships of other types of reactions and catalysts.
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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
The main parts of the proposed research have been successfully completed in advance, with the two most important papers from this research published in top journals in chemistry, proving the concepts and hypotheses of the proposal: J. Am. Chem. Soc., 2024, 146, 3210; Chem. Sci., 2024, 15, 5123 (the PI is the Last and Corresponding Author of these publications). In particular, we have successfully provided key understandings of the pH-dependency of M-N-C catalysts observed from experiments. We also developed new computational methodologies and tools for electrochemistry analyses, such as the pH- and reversible hydrogen electrode-dependent surface Pourbaix diagrams (Langmuir, 2024, 40, 7632) and the digital platform for microkinetic modeling (CatMath; Front. Chem. Sci. Eng., 2023, 17, 2156).
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今後の研究の推進方策 |
In the next step, we will analyze the recently emerging M-N-C dual-atom catalysts (DACs) in detail, in particular for ORR. We will combine advanced characterization techniques with our microkinetic modeling, to fully analyze the surface coverage effects of DACs under electrochemical conditions and the structure-performance relationships of DACs. Finally, we will develop reliable design guidelines for high-performance M-N-C catalysts in various industrially important reactions.
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