| Project/Area Number |
23K13703
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| Research Category |
Grant-in-Aid for Early-Career Scientists
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| Allocation Type | Multi-year Fund |
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| Review Section |
Basic Section 32010:Fundamental physical chemistry-related
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| Research Institution | Tohoku University |
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Principal Investigator |
LI HAO 東北大学, 材料科学高等研究所, 准教授 (50967198)
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| Project Period (FY) |
2023-04-01 – 2025-03-31
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| Project Status |
Granted (Fiscal Year 2023)
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| Budget Amount *help |
¥4,680,000 (Direct Cost: ¥3,600,000、Indirect Cost: ¥1,080,000)
Fiscal Year 2024: ¥1,300,000 (Direct Cost: ¥1,000,000、Indirect Cost: ¥300,000)
Fiscal Year 2023: ¥3,380,000 (Direct Cost: ¥2,600,000、Indirect Cost: ¥780,000)
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| Keywords | Catalysis theory / Electrocatalysis / M-N-C catalysts / Single-atom catalysts / Microkinetic modeling / pH-dependent simulation / Electric field effects / Oxygen reduction / pH effects |
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| Outline of Research at the Start |
The pH and field effects on the oxygen reduction performance of M-N-C catalysts will be unveiled, and new catalysts (e.g., M-N-C catalysts with new local atomic structure and heterogeneous molecular catalysts) will be designed and screened based on the theory developed by this project.
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| Outline of Annual Research Achievements |
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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| Current Status of Research Progress |
Current Status of Research Progress
1: Research has progressed more than it was originally planned.
Reason
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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| Strategy for Future Research Activity |
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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