It is well known that ammonia is produced through a catalytic reaction at high temperature and pressure from pure nitrogen and hydrogen. This catalytic chemical process is a massive and high-energy-consuming process, but a very important one for nitrogen fixation. Here, we show a non-catalyzed one-step synthesis of ammonia from atmospheric air (nitrogen source) and water (hydrogen source), based on an interfacial reaction between the air plasma gas phase and the water phase, at 25 °C and atmospheric pressure. In the plasma/liquid interfacial reaction (P/L reaction), atomic nitrogen in both air plasma and nitrogen plasma first abstracts hydrogen from the water phase surface at the P/L interface, and then NH is produced without any catalyst. Transiently formed NH is reduced further at the water phase, affording NH3, which then dissolves in the water phase. The P/L reaction may provide an alternative solution that enables both energy conservation and CO2 emission reduction.
Cu-Sn alloy electrodes were prepared by simple electrodeposition method for the electrochemical reduction of CO2 into CO and HCOO−. The alloy electrode surfaces provided good selectivity and efficiency in electrochemical CO2 conversion because they provided appropriate binding energies between the metal and the reactive species obtained through CO2 reduction. Therefore, product selectivity can be modulated by altering the Cu-Sn crystal structure of the electrode. Using the Cu-Sn alloy electrodes, electrochemical reduction was performed at applied potentials ranging from − 0.69 to − 1.09 V vs. reversible hydrogen electrode (RHE). During electrochemical CO2 reduction, all the prepared Cu-Sn alloy electrodes showed prominent suppression of hydrogen evolution. In contrast, Cu87Sn13 has high selectivity for CO formation at all the applied potentials, with maximum faradaic efficiency (FE) of 60% for CO at − 0.99 V vs. RHE. On the other hand, Cu55Sn45 obtained a similar selectivity for electrodeposition of Sn, with FE of 90% at − 1.09 V vs. RHE. Surface characterization results showed that the crystal structure of Cu87Sn13 comprised solid solutions that play an important role in increasing the selectivity for CO formation. Additionally, it suggests that the selectivity for HCOO− formation is affected by the surface oxidation state of Sn rather than by crystal structures like intermetallic compounds. The Cu-Sn alloy catalysts prepared by simple electrodeposition can control the selectivity for CO and HCOO− formation by tuning its crystal structure. Surface analyses revealed that solid solutions and the oxidation state of Sn play an important role in the formation of CO and HCOO− upon CO2 reduction, respectively.
An interfacial reaction between the UV irradiated water phase (H˙ provides) and the electron-discharged nitrogen-gas phase (N atom provides) produces ammonia efficiently.