Steering from electrochemical denitrification to ammonia synthesis

Huan Li, Jun Long, Huijuan Jing and Jianping Xiao ()
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Huan Li: Chinese Academy of Sciences
Jun Long: Chinese Academy of Sciences
Huijuan Jing: Chinese Academy of Sciences
Jianping Xiao: Chinese Academy of Sciences

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract The removal of nitric oxide is an important environmental issue, as well as a necessary prerequisite for achieving high efficiency of CO2 electroreduction. To this end, the electrocatalytic denitrification is a sustainable route. Herein, we employ reaction phase diagram to analyze the evolution of reaction mechanisms over varying catalysts and study the potential/pH effects over Pd and Cu. We find the low N2 selectivity compared to N2O production, consistent with a set of experiments, is limited fundamentally by two factors. The N2OH* binding is relatively weak over transition metals, resulting in the low rate of as-produced N2O* protonation. The strong correlation of OH* and O* binding energies limits the route of N2O* dissociation. Although the experimental conditions of varying potential, pH and NO pressures can tune the selectivity slightly, which are insufficient to promote N2 selectivity beyond N2O and NH3. A possible solution is to design catalysts with exceptions to break the scaling characters of energies. Alternatively, we propose a reverse route with the target of decentralized ammonia synthesis.

Date: 2023
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DOI: 10.1038/s41467-023-35785-w

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