電気化学的CO2還元による電解燃料製造のための適切な触媒に関する研究

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🔬研究者:TMCN触媒のCO2RR/CORR活性をDFTで比較した初の系統的データセットとして、触媒設計研究の出発点になる。

🏢実務担当者:電解燃料・e-fuel事業の触媒選定や技術ロードマップ検討の基礎的知見として参照可能。

🏛政策担当者:CO2資源化・電解燃料分野への研究開発投資判断の背景資料として活用できる。

Current global energy and environmental challenges can be viewed as the interaction of three connected factors: the use of fossil fuels, carbon dioxide (CO2) emissions, and global warming. The global energy landscape remains largely dependent on fossil fuels, leading to substantial CO2 emissions and disturbing the climatic equilibrium. Nonetheless, one promising strategy for addressing this challenge is to regard CO2 as a resource, thereby converting the challenge into an opportunity for ecological restoration through the use of CO2 for the production of sustainable fuels. This approach turns CO2 into eco-friendly, value-added compounds, promoting greenhouse gas reduction and sustainable energy development. An effective solution to these limitations can possibly be addressed through chemical physics and electrochemistry, particularly through the implementation of the electrochemical CO2 reduction reaction (CO2RR), which converts CO2 into several single and multi-carbon (C1/C2 products) compounds, including carbon monoxide, formic acid, methanol, methane, methanediol, ethylene, ethane, and ethanol. This process can be readily integrated with current renewable energy infrastructure, enabling the coupling of CO2 conversion with sustainable power sources and therefore storing renewable energy as chemical products. However, their practical application remains limited by the low catalytic activity, poor selectivity, and broad product distribution of conventional metal catalysts. In several instances, these catalysts primarily convert CO2 to only CO or formic acid with relative simplicity, whereas the synthesis of more reduced or multi-carbon compounds requires more energy input and often exhibits restricted efficiency. Hence, the electrochemical CO reduction reaction (CORR) may provide essential solutions to tackle the current challenges in the field of CO2RR. Thus, this Ph.D. thesis is dedicated to the exploration of these two research directions to identify more efficient and selective reaction pathways for sustainable carbon transformation via both CO2RR and CORR. To the best of our knowledge, this thesis presents the first systematic computational investigation of transition metal carbonitrides (TMCNs) for electrochemical CO2RR and CORR. A rigorous computational framework using density functional theory (DFT) within the Vienna Ab initio Simulation Package (VASP) was applied to analyze these surfaces for both CO2RR and CORR. This theoretical study examined 33 different catalytic surfaces, eleven TMCNs in (100), (111), and (110) facets, to predict their catalytic activity towards the formation of C1 and C2 products. Moreover, comprehensive computational evaluations were performed to assess the behavior of these different TMCNs in diverse electrochemical environments with pre-adsorbed CO surface coverage. The catalytic performance was investigated using the conventional and the Mars-van Krevelen (MvK) mechanisms and over 2000 reaction pathways to identify the most thermodynamically favorable routes and predict the best TMCN candidate(s) for efficient carbon conversion and management. In the catalytic activity analysis, TMCN(110) was identified as offering the highest activity for both CO2RR and CORR via the MvK mechanism. In conventional pathways, TMCN(111) was found to be the most active for CO2RR, while TMCN(100) was the best for CORR, and TMCN(111) was inactive toward conventional CORR. Overall, this dissertation provides a comprehensive theoretical assessment of TMCNs and offers computationally grounded predictions for their potential use in converting carbon into green fuels, thereby addressing important environmental and sustainable energy concerns.

• openalex https://hdl.handle.net/20.500.11815/8490first seen 2026-10-24 04:39:44 · last seen 2026-11-01 04:34:01