Proceedings of MATSUS Fall 2024 Conference (MATSUSFall24)
Publication date: 28th August 2024
The electrochemical nitrate reduction reaction (NO3RR) is a promising approach for the conversion of nitrate contaminants into ammonia (NH3), a desirable chemical nowadays produced with the energy-intensive Haber Bosch process.1-3 Cu remains one of the most effective catalysts for NO3RR.1-3 However, the structural and compositional characteristics of Cu catalysts that tune NH3 selectivity and production rates are poorly understood, which limits further advancements of this field.1-3
Herein, we use a library of well-defined and shaped tunable Cu and Cu oxide nanocrystals to study the impact of size, shape and composition of Cu catalysts on NH3 selectivity and production rate with the goal of outperforming the current state of the art for NH3 generation. We find that the NH3 production rate follows the trend: 10 nm Cu spheres ˃ Cu2O cubes ˃ metallic Cu cubes ˃ other sizes of Cu spheres. Interestingly, the 10 nm Cu spheres and the Cu2O cubes undergo more pronounced morphological changes during NO3RR. These changes in morphology suggest that the initial size, shape and composition of Cu catalysts impacts the dynamic evolution in Cu coordination environment and oxidation state in a way that ultimately determines the optimal NH3 yield for the 10 nm Cu spheres. We use a miscellanea of techniques, including electron microscopy and X-ray absorption spectroscopy, etc., to elucidate the emerged structure/composition/reactivity relationships for the entire Cu catalyst library. Based on this understanding, we propose a state of the art Cu catalyst for NO3RR with competing NH3 selectivity and production rate.
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