Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.245
Publication date: 18th July 2023
Ammonia (NH3), being the basis of all nitrogen fertilizers, constitutes one of the pillars of modern society, without which nearly half of the population would not be present on Earth.1 Furthermore, thanks to its properties (high energy content and density), it is recently emerging as a backbone fuel towards decarbonisation.2 Up-to-date, NH3 is mainly produced via the energy-intensive Haber-Bosch process and, to meet the future NH3 demand, new green synthesis techniques need to be developed.3
To this end, electrochemical nitrogen and nitrate reduction reactions (E-NRR and E-NO3RR) have received considerable attention since, among other advantages, they permit the utilization of electricity from renewables. Also, taking into account that molybdenum and sulphur play key roles in nitrogenase-based nitrogen fixation, molybdenum disulphide (MoS2) is expected to be active toward E-NRR, even if it has already demonstrated good catalytic activity toward hydrogen evolution reaction (HER, the main competitor of E-NRR).4
In this work, MoS2 has been tested for E-NRR and E-NO3RR in combination with different formulated electrolytes (LiSO4 and K2SO4 at different concentrations and pH values). A flow cell with a gas diffusion electrode, on which the catalyst is immobilized through air-brushing technique, has been used to perform all the experiments. Regarding E-NRR, encouraging results were obtained when employing Li+ as an additive in the electrolyte, leading to Faradaic efficiencies between 5 and 10%, as well as 85-301 μmol g-1 h-1 yield at -0.6 V vs. RHE. Further, since NH3 was detected not only in the cathodic site, but also in the anodic one, as well as absorbed within the cationic membrane, the interactions between the Nafion membrane and NH3 were also studied, observing that NH3 adsorption decreased when the size of the cation raised (around 60% of NH3 was absorbed when employing Li2SO4, ca. 20% when employing K2SO4).
Finally, in the case of NO3RR, design of the experiment and surface response methodology (DoE/RSM) were employed to gain further insight onto the influence of operational conditions (potential, catalyst loading and salt concentration in the electrolyte) on the Faradaic efficiency and NH3 yield of the NO3RR, as well as the possible interaction between those parameters.
S. Garcia-Ballesteros wants to thank the Politecnico di Torino for the Starting grant RTDA
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