Post Nitrogen Electrocatalysis Era From Li–N₂Batteries to Zn–N₂Batteries

Abstract

ability to deliver high energy density with good environmental friendliness, which are considered as the promising devices for energy storage and conversion in the sustainable human society. [1] Considering the abundance of nitrogen resource in the air, scientists began to shift their research perspective from O 2 or CO 2 to N 2 . With the first presentation of the concept for the Li-N 2 battery in 2017, [2] a new device combining energy conversion and N 2 fixation starts to come into sight. Inspired by this new model, from organic Na/Al-N 2 batteries [3] to aqueous Al/Zn-N 2 batteries, [4] other types of metal-N 2 batteries began to be reported as illustrated in Figure 1. For realizing electrochemical NH 3 production, the reaction path is nitrogen reduction reaction (NRR) during the discharge process for both organic and aqueous metal-N 2 batteries. Based on diverse reaction mechanism under aqueous and organic solution, the subsequent reaction in the charge process for two types of metal-N 2 batteries is different, that is, the nitrogen extraction reaction (NER) for the organic ones and oxygen evolution reaction (OER) for the aqueous ones. Overall, the developments of aqueous metal-N 2 batteries are mainly inspired by the organic metal-N 2 batteries and lag behind their development. Up to now, only part of the reported metal-N 2 batteries shows good electrochemical reversibility, [5] while some are electrochemical irreversible primary batteries that can only be discharged. [6] Unlike organic metal-N 2 batteries, for all the reversible/irreversible aqueous metal-N 2 batteries, NH 3 would be generated during the discharging process. In the meantime, these reversible aqueous metal-N 2 batteries can still be recharged even after the NH 3 releasing. [7] NH 3 plays an important role in maintaining the survival of human beings and the sustainable development for the social economy. First, NH 3 is an important chemical raw material for the production of agricultural nitrogen fertilizer, as well as a key energy storage intermediate and carbon-free energy carrier for the production of fuels, dyes, and other industries articles. [8] Moreover, NH 3 is considered as an excellent hydrogen energy carrier because of its high hydrogen content without carbon element and easy liquefaction for storing and transporting. [9] However, the industrial NH 3 synthesis is still carried out via the Haber-Bosch process developed 100 years ago based on the reaction of N 2 +3H 2 →NH 3 , which proceeds under high working pressure of 20 MPa and heat temperature of 673 K, resulting in Metal-N 2 batteries attract considerable research attention due to the dualfunctional characteristics applied in energy storage and conversion, as well as electrochemical artificial NH 3 yield. Nonetheless, it has been found that not all kinds of metal-N 2 batteries are suitable for combining the above two applications. Herein, recent advances in metal-N 2 batteries are summarized. First, the electrochemical reaction mechanisms for all types of metal-N 2 batteries,...

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