Abstract
NH3 is an essential nutrient for life, but its production through anthropogenic N2-fixing process has caused alarming damages to ecosystems and human health. Excessive NO3 - leakage into water bodies due to overfertilization has led to the formation of "dead zones" in coastal areas. Denitrification generates N2O, which is 300 times more potent than CO2. Restoring the balance between the generation and elimination of Nr is an urgent task for humanity. Efforts to address the negative impact of human-generated Nr have focused on converting it to harmless N2 or improving its utilization in the nitrogen cycle. One promising method is electrochemical conversion, which can eliminate Nr without additional oxidants/reductants. However, achieving selective NO3RR toward N2 is challenging. An alternative approach is to convert other forms of Nr to NH3 in an electrochemical reactor, which could reduce the environmental impact of Nr and decrease the NH3 demand from the Haber-Bosch process, while also reducing the use of fossil-derived H2.In this work, we report our work on the development of a membrane-free alkaline electrolyzer (MFAEL), which transforms Nr into NH3 as the sole N-containing product. With the inexpensive and robust MFAEL system, we achieved an ampere-level partial current density towards NH3 production. By properly choosing the conditions of NH3 collection from MFAEL, continuous production of pure NH3-based chemicals can be realized without the need for additional separation procedures. Techno-economic analysis (TEA) suggests the potential economic feasibility of the waste-to-NH3 process by coupling electrodialysis (ED) for Nr concentration and the MFAEL process for Nr conversion, offering an all-sustainable route for upcycling waste N into the highest-demanded N-based chemical product. Our recent efforts on green-ammonia capture CO2 and reduction to valuable chemicals will also be briefly presented.
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