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The proposed work is in response to R3 Appendix E research topic “Conversion of CO2 into Fuel.” The space mission of NASA for Mars will require sufficient amounts of fuels for the exploration of the planet and the return of samples or humans to Earth. For this, the development of an in-situ, efficient method to synthesize fuels from the resources abundant on Mars is critical. This proposal aims to develop efficient, selective, and durable electrocatalysts for CO2 reduction by developing atomically dispersed metal atoms incorporated in high-surface-area carbon nano-onions (CNOs). If successful, this research will pave a way to efficient and economic conversion of CO2 (the most abundant gas (95 %) in the atmosphore of the Mars) into valuable chemicals and fuels such as such as methane, methanol, ethanol, formate, and syngas. This proposal is based on several innovative concepts:(i) economic and tailorable use of metal atoms atomically dispersed in support for catalyst design, (ii) stablized and abundant immobilization of atomically dispersed catalytic metals by coordination with nitrogen (N), and (iii) enhanced reactivity and abundance of metal-N4 sites by the high curvature of CNO support, that will creae active sites for CO2 reduction reaction (CO2RR). We will establish synthetic methods to modify CNOs by incorporating heteroatoms and subsequent addition of metallic ions (see Figure 1). The active sites formed by this approach will create asymmetric charges on the electrode surface and will facilitate the adsorption of CO2 reactants, thereby will lower the kinetic barrier of CO2 reduction pathway. Through systematic synthesis, structure analyses, electrochemical characterizations, and computational modeling, knowledge will be gained on structure-property-activity relations of catalysts.
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