Electrocatalytic Oxidation of Ammonia to Nitrogen Oxides in Liquid Ammonia

在第一个供资期开发的高压电池的基础上，该项目的重点将从基本完成的甲烷氧化转移到电化学氨氧化工艺。氢应在阴极析出，而氮氧化物应在阴极产生，硝酸盐应最终从阴极获得。这可以将联合收割机结合起来，一方面，在氨支持的氢基础设施的情况下从氨中有效释放氢，另一方面，生产氮肥。因此，氨的阳极氧化将取代奥斯特瓦尔德工艺。这一过程可能是未来能源系统中一个令人感兴趣的要素，因为未来的能源系统可能部分依赖氨作为能源载体。(1)在第一个供资期间建造的电化学高压池必须加以改造，以便能够用于处理液氨。(2)必须开发适当的分析技术来分析阳极室。(3)必须找到能在液氨中稳定阴极析氢的电极材料。(4)必须找到当含氧化合物存在于阳极侧的液氨中时氮氧化物以高选择性形成的阳极材料。(5)整个系统必须通过检查广泛的参数来全面表征其性能。(6)与在液氨中的反应相比，氨在水环境中的氧化电化学分解过程中的行为将被研究。该项目的成功完成将为在不寻常的反应介质中进行不寻常的反应提供基本的见解，但也可以为替代传统肥料生产奠定基础。

Based on the high-pressure cell developed in the first funding period, the focus of the project will move away from methano oxidation in oleum, which is essentially completed, to a process for electrochemical ammonia oxidation. Hydrogen shall be evolved at the cathode, while nitrogen oxides are to be produced cathodically, from which nitrates should ultimately be accessible. This could combine, on the one hand, the efficient release of hydrogen from ammonia in the context of an ammonia-supported hydrogen infrastructure and, on the other hand, the production of nitrogen fertilizer. The anodic oxidation of ammonia would thus replace the Ostwald process. Such a process could be an interesting element in a future energy system, which could partly rely on ammonia as energy vector.To achieve this overall goal, six sub-objectives must be achieved. (1) The electrochemical high-pressure cell constructed during the first funding period must be modified so that it can be used to work with liquid ammonia. (2) Appropriate analytical techniques must be developed for analysis of the anode compartment. (3) Electrode materials must be found on which hydrogen can be stably evolved cathodically in liquid ammonia. (4) Anode materials must be found at which nitrogen oxides are formed with high selectivity when oxygen-containing compounds are present in the liquid ammonia on the anode side. (5) The overall system must be comprehensively characterized in terms of its performance by examining a wide range of parameters. (6) As a comparison to the reaction in liquid ammonia, the behavior of ammonia during oxidative electrochemical decomposition is to be investigated in aqueous environment. Successful completion of this project would both provide fundamental insight in an unusual reaction in an unusual reaction medium, but could also lay the foundations for an alternative to conventional fertilizer production.