Amorphousnanoparticles for the electrocatalytic reduction of CO 2 into added-value chemicals Nivetha Jeyachandran, Wangchao Yuan, Xiang Liand Cristina Giordano Department of Chemistry, Queen Mary University of London, Mile End Road, London, E1 4NS, UK The increasing levels of CO 2 has raised growing concerns to our environment and reducing the level of CO 2 emissions is not practically feasible with the growing human population. One attractive strategy is the conversion of CO 2 into added value chemicals that can be used for further useful applications. CO 2 is a stable molecule, and its electrochemical reduction requires a suitable catalyst. Metal-based catalysts have been largely investigated for CO 2 RR, and although promising, the difficulty achieving a high selectivity and faradaic efficiency towards specific products, especially hydrocarbons, is still a challenge, alongside the concern over cost, stability, and scarcity of some metal catalyst. 1 Recently, research is focusing towards amorphous, rather than crystalline, catalysts, for their isotropic nature is expected to impart superior performance towards CO 2 RR originating from the disorder within the structure and loose bonds between atoms. 2 Our current research focuses on tuning the crystallinity of Cu nanoparticles via a green, cost-friendly, and facile method, called the urea glass route. 3,4 Remarkably, the incorporation of a selected nitrogen-carbon rich source (namely, 4,5 dicyanoimidazole) at low temperatures allow the formation of amorphous Cu, whilst a second thermal treatment enables the transformation to crystalline Cu 0 . We found that the combination of surface Cu 0 and Cu 1+ (observed via XPS studies) present in our amorphous and crystalline Cu nanoparticles leads to interesting differences in the final catalytic activity when tested under CO 2 reaction conditions. 5 References 1. N. Jeyachandran, W. Yuan and C. Giordano, Cutting-Edge Electrocatalysts for CO2RR, Molecules , 2023, 28 , 3504. 2. Y.-X. Duan, F.-L. Meng, K.-H. Liu, S.-S. Yi, S.-J. Li, J.-M. Yan and Q. Jiang, Amorphizing of Cu Nanoparticles toward Highly Efficient and Robust Electrocatalyst for CO2 Reduction to Liquid Fuels with High Faradaic Efficiencies, Advanced Materials , 2018, 30 , 1706194. 3. C. Giordano, C. Erpen, W. Yao, B. Milke and M. Antonietti, Metal Nitride and Metal Carbide Nanoparticles by a Soft Urea Pathway, Chem. Mater. , 2009, 21 , 5136–5144. 4. W. Yuan, N. Jeyachandran, T. Rao, A. Ghulam Nabi, M. Bisetto, D. Di Tommaso, T. Montini and C. Giordano, Study on the Structure vs Activity of Designed Non-Precious Metal electrocatalysts for CO2 Conversion, Materials Letters , 2023, 341 , 134167. 5. N. Jeyachandran, W. Yuan, X. Li, A. Muthuperiyanayagam, D. Di Tommaso and C. Giordano, Tuning the Crystallinity of Cu- based electrocatalysts: Synthesis, Structure, and Activity towards the CO2 Reduction Reaction, submitted .
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