澳大利亚莫纳什大学Simonov Alexandr N.团队开发了几乎100%电流-氨效率的氮电还原策略。相关研究成果发表在2022年7月22日出版的《自然》。
除用于化肥和化学工业外，氨目前被视为碳基燃料的潜在替代品，并被视为全球可再生能源运输的载体。要实现这一愿景，就需要将现有的以化石燃料为基础的NH3生产技术转变为更简单、规模灵活的技术，例如电化学锂介导的氮还原反应（Li-NRR）。其提供了从N2到氨的真正途径，但受到有限的产率和效率的阻碍。
该文中，研究人员研究了电解质在该反应中的作用，并提出了一种通过电极-电解质界面区域的紧密离子层实现的高效、稳健的过程。该界面由高浓度酰亚胺基锂盐电解质生成，使稳定的氨产率达到150±20 nmol s-1 cm-2，电流-氨效率接近100%。在电极表面形成的离子组装抑制电解质分解并支持稳定的N2还原。该研究强调了锂NRR性能与电极-电解质界面物理化学性质之间的相互关系。
研究结果将指导开发稳健、高效的可持续氨生产工艺。
附：英文原文
Title: Electroreduction of nitrogen at almost 100% current-to-ammonia efficiency
Author: Du, Hoang-Long, Chatti, Manjunath, Hodgetts, Rebecca Y., Cherepanov, Pavel V., Nguyen, Cuong K., Matuszek, Karolina, MacFarlane, Douglas R., Simonov, Alexandr N.
Issue&Volume: 2022-07-22
Abstract: Beyond its use in the fertiliser and chemical industries1, ammonia is currently seen as a potential replacement for carbon-based fuels and as a carrier for worldwide transportation of renewable energy2. Implementation of this vision requires transformation of the existing fossil fuel based technology for NH3 production3 to a simpler, scale-flexible technology, such as the electrochemical lithium-mediated nitrogen reduction reaction (Li-NRR)3,4. This provides a genuine pathway from N2 to ammonia, yet is hampered by limited yield rates and efficiencies4-12. Here we investigate the role of the electrolyte in this reaction and present a high-efficiency, robust process enabled by compact ionic layering in the electrode-electrolyte interfacial region. The interface is generated by a high-concentration imide-based lithium salt electrolyte, enabling stabilised ammonia yield rates of 150±20 nmol s-1 cm-2 and current-to-ammonia efficiency closely approaching 100%. The ionic assembly formed at the electrode surface suppresses electrolyte decomposition and supports stable N2 reduction. Our study highlights the interrelation between the performance of the Li-NRR and the physicochemical properties of the electrode-electrolyte interface. We anticipate that these findings will guide the development of a robust, high-performance process for sustainable ammonia production.
DOI: 10.1038/s41586-022-05108-y
Source: https://www.nature.com/articles/s41586-022-05108-y