Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.176
Publication date: 18th July 2023
With 170 MT produced in 2020, ammonia is one of the most produced chemicals in the world [1]. However, it is currently produced using the Haber-Bosch process which contributes >1 % of global CO2 emissions. Continuous electrochemical nitrogen Reduction Reaction may not be able to completely replace the Haber-Bosch process but it has numerous advantages which may secure its place in green ammonia production. Continuous electrochemical nitrogen reduction reaction can be done at ambient pressures and temperatures, run directly from (renewable) electricity and enables ammonia production in smaller decentralised facilities. However, research into this field is still relatively new, performance is unoptimised and many important scientific questions remain unanswered. In particular, efficiency and current density are too low for commercial application and the key mechanisms by which the reaction occurs are still unknown. Recently, there have been significant advances which have focused on electrolyte optimisation [2-3] and cell design [4].
Optimising performance through the use of dynamic operating conditions is attractive because it can be done at little extra cost while achieving substantial improvements. Dynamic operating conditions have already been demonstrated to increase activity and selectivity towards desired products in the electrochemical CO2 Reduction Reaction [5-6] and increase electrode stability in electrochemical [7].
In this work, dynamic operating conditions are investigated in the continuous electrochemical nitrogen reduction system using Electrochemistry-Mass Spectrometry, a technique which allows subsecond detection of gases and volatile species in real-time. This work builds on Krempl et al.’s work by improving detection times reducing noise which allows dynamic conditions to be investigated [8]. By monitoring H2 evolution (a key parasitic product) at different voltages, the point at which it is minimised was found. However, operating at this new optimal led to the accumulation of a reaction intermediate (lithium) which was not reacting quickly enough to form ammonia. Dynamic operating conditions were utilised to alternate between this H2 evolution minimum and an ammonia forming maximum. With this combination, ammonia selectivity was found to increase substantially from 7.9 % to 18 %.
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