Xu Yuan-Zi, Dürr Robin N, Häfliger Florian, Abbott Daniel F, Mougel Victor
Department of Chemistry and Applied Biosciences, ETH Zürich, Zürich, Switzerland.
Angew Chem Int Ed Engl. 2025 Jul 28;64(31):e202504174. doi: 10.1002/anie.202504174. Epub 2025 Jun 23.
The electrochemical reduction of nitrate (NO₃RR) offers a promising route for decentralized and sustainable ammonia production while addressing environmental challenges associated with nitrate pollution. However, the development of practical implementations has been slowed by the challenge of creating highly stable and selective catalysts for strongly basic environments, along with the difficulty of efficiently recovering ammonia from dilute solutions. Here, we introduce a partially oxidized amorphous iron-phosphide (POA-FeP) electrocatalyst that combines high activity and stability with an innovative Joule-stripping strategy for ammonia recovery. Electrodeposited onto nickel foam (NF), the POA-FeP catalyst achieves benchmark partial current densities of -720 mA cm in neutral media and -932 mA cm in alkaline media, and near quantitative Faradaic efficiencies (FE). The robustness of the POA-FeP/NF catalyst was highlighted by its ability to maintain FE above 90% during continuous operation for over 1000 h at a total current density of -300 mA cm. We demonstrate that the Joule heating resulting from the operation of the electrolyzer at high current density can be exploited to induce the volatilization of ammonia, which can then be recovered as solid ammonium chloride with >95% yield. This integrated Joule-stripping approach simplifies ammonia recovery and opens up new possibilities for scalable and energy-efficient nitrate reduction systems.
硝酸盐的电化学还原(NO₃RR)为分散式可持续制氨提供了一条有前景的途径,同时解决了与硝酸盐污染相关的环境挑战。然而,由于要为强碱性环境制备高度稳定且具选择性的催化剂存在挑战,以及从稀溶液中高效回收氨存在困难,实际应用的发展受到了阻碍。在此,我们介绍一种部分氧化的非晶态铁磷化物(POA-FeP)电催化剂,它将高活性和稳定性与用于氨回收的创新焦耳汽提法相结合。POA-FeP催化剂电沉积在泡沫镍(NF)上,在中性介质中实现了-720 mA cm的基准分电流密度,在碱性介质中实现了-932 mA cm的基准分电流密度,以及近乎定量的法拉第效率(FE)。POA-FeP/NF催化剂的稳健性体现在其在-300 mA cm的总电流密度下连续运行超过1000小时期间能够将FE维持在90%以上。我们证明,电解槽在高电流密度下运行产生的焦耳热可用于诱导氨的挥发,然后氨可以以>95%的产率回收为固体氯化铵。这种集成的焦耳汽提方法简化了氨回收,并为可扩展且节能的硝酸盐还原系统开辟了新的可能性。