In situ evolution of Sn/Cu2O heterostructure catalysts for modulating selectivity in electrosynthesis of ammonia and urea
)Graphical Abstract
Abstract
Electrocatalytic nitrate reduction reaction (NO3−RR) and its coupling with CO2 could provide new sustainable pathways for the synthesis of ammonia and urea, respectively. However, their practical applications are hindered by the lack of catalysts with satisfied Faraday efficiency and yield. Herein, we report self-supported electrochemically reconstituted Sn/Cu2O bifunctional catalysts for the efficient synthesis of ammonia and urea. In the NO3−RR, Sn/Cu2O-β catalysts electrodeposited for 800 s provided an excellent ammonia yield of 0.496 mmol·h−1·cm−2 and Faraday efficiency of 98.5%. Besides, Sn/Cu2O-α catalysts electrodeposited for 400 s achieved the maximum Faraday efficiency of 13.5% and outstanding urea yield of 32.35 μmol·h−1·cm−2 in C–N coupling. Comprehensive analyses confirm that bi-selectivity to ammonia and urea synthesis could be achieved by modulating the chemical state of Cu in Sn/Cu2O catalysts, these results are superior to most reported transition metal-based catalysts in synthesis of urea and/or ammonia. In situ Fourier transform infrared (FTIR) spectroscopy revealed that *CONH2 intermediates are essential for urea synthesis. This work will provide a feasible strategy for the development of bifunctional electrocatalysts for efficient ammonia and urea synthesis.
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References
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