Abstract
Lithium-mediated ammonia electrochemical synthesis (LMAES) holds promise for approximating and superseding the capacity of Haber-Bosch technology. However, currently used tetrahydrofuran electrolyte in such system hinders the further enhancement of nitrogen fixation performance greatly due to the over-passivation of the reaction interface suppressing the corrosion rate of the active species on metallic lithium. Here, we develop a remarkably 1,2-diethoxyethane (DEE) electrolyte to enhance the performance of LMAES. Systematic simulations combined with experimental results jointly elucidate that the unique Li+ solvation environment in DEE electrolyte significantly weakens the passivation of the electrode interface and triggers the general corrosion behavior of active species to electrodeposited lithium. Compared with conventional tetrahydrofuran electrolyte, this DEE electrolyte brings nearly twice the improvement of Faradaic efficiency (from 33.4 % to 61.7 %). This work offers a progressive insight into advanced electrolyte designs for LMAES.
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