High Efficiency Electrochemical Nitrogen Fixation Achieved with a Lower Pressure Reaction System by Changing the Chemical Equilibrium.

ABSTRACT

We demonstrate a simple and effective chemical equilibrium regulation strategy to improve the efficiency of electrochemical ammonia synthesis by constructing electrochemical reaction system that works at significantly lower pressure than the Haber-Bosch process. Transferring the nitrogen reduction reaction from ambient conditions to a lightly pressurized environment not only accelerates the activation of the N≡N triple bond but also inhibits the competing reaction of hydrogen evolution while promoting the dissolution and diffusion of nitrogen. The verification experiment of using well-designed Fe3 Mo3 C/C composite nanosheets as the nitrogen reduction catalyst shows that the lower pressure reaction system can improve the Faradaic current efficiency by one order of magnitude. Moreover, the comparatively low-pressure reaction system can greatly reduce the cell voltage of the ammonia synthesis reaction (up to 33 %) even at the relatively low pressure of 0.7 MPa, which is of significance for decreasing the energy consumption of electrochemical ammonia synthesis under mild conditions.