氨作为一种无碳绿色燃料以及重要的工农业原料,在日常生活中发挥了巨大的作用。目前,氨的工业生产主要通过哈伯–博施法进行,这一工艺过程需要高温高压严苛的反应条件,在消耗大量化石燃料的同时也给环境带来了极大的负担。电催化氮还原...氨作为一种无碳绿色燃料以及重要的工农业原料,在日常生活中发挥了巨大的作用。目前,氨的工业生产主要通过哈伯–博施法进行,这一工艺过程需要高温高压严苛的反应条件,在消耗大量化石燃料的同时也给环境带来了极大的负担。电催化氮还原合成氨(NRR)方法由此崭露头角,其在常温常压的温和条件下以氮气和水为原料,以可持续能源(太阳能、风能等)发电为驱动力合成氨,可以实现绿色、零排放的预期效果。然而,在研究过程中始终存在以下三个问题,一是氮气化学性质稳定,N≡N键断裂需要较大的能量;二是在常用的水系电解液中倾向于发生较强的析氢反应(HER),使电催化氮还原的选择性较低;三是由于氮气在水中的溶解度低,扩散动力学缓慢,反应界面氮气供应不足。因此,针对这三种科学问题,从电催化剂、电解液及工作电极的角度出发,探索并设计有效的优化方案,对进一步推进电催化氮还原反应的实际应用具有重要意义。As a carbon free green fuel and an important industrial and agricultural raw material, ammonia plays a huge role in daily life. At present, the industrial production of ammonia is mainly carried out through the Haber Bosch process, which requires harsh reaction conditions of high temperature and high pressure. Thus, this process consumes a large amount of fossil fuels, and also brings great burden to the environment. The method of electrocatalytic nitrogen reduction (NRR) to synthesize ammonia has temporarily emerged. It synthesizes ammonia using nitrogen and water as raw materials under mild conditions of normal temperature and pressure, driven by sustainable energy sources such as solar and wind power, and can achieve the expected effects of green and zero emissions. However, it is found that the following three problems always exist in this process. First, the chemical property of nitrogen is stable, N≡N fracture requires a large energy. Second, in commonly used aqueous electrolytes, strong hydrogen evolution reaction (HER) tends to occur, resulting in lower selectivity for NRR. Third, due to the low solubility and slow diffusion of nitrogen in water, nitrogen supply at the reaction interface is always insufficient. Therefore, exploring and designing effective optimization schemes from the perspectives of electrocatalysts, electrolytes, and working electrodes for these three scientific issues is of great significance for further promoting the practical application of electrocatalytic nitrogen reduction reactions.展开更多
文摘氨作为一种无碳绿色燃料以及重要的工农业原料,在日常生活中发挥了巨大的作用。目前,氨的工业生产主要通过哈伯–博施法进行,这一工艺过程需要高温高压严苛的反应条件,在消耗大量化石燃料的同时也给环境带来了极大的负担。电催化氮还原合成氨(NRR)方法由此崭露头角,其在常温常压的温和条件下以氮气和水为原料,以可持续能源(太阳能、风能等)发电为驱动力合成氨,可以实现绿色、零排放的预期效果。然而,在研究过程中始终存在以下三个问题,一是氮气化学性质稳定,N≡N键断裂需要较大的能量;二是在常用的水系电解液中倾向于发生较强的析氢反应(HER),使电催化氮还原的选择性较低;三是由于氮气在水中的溶解度低,扩散动力学缓慢,反应界面氮气供应不足。因此,针对这三种科学问题,从电催化剂、电解液及工作电极的角度出发,探索并设计有效的优化方案,对进一步推进电催化氮还原反应的实际应用具有重要意义。As a carbon free green fuel and an important industrial and agricultural raw material, ammonia plays a huge role in daily life. At present, the industrial production of ammonia is mainly carried out through the Haber Bosch process, which requires harsh reaction conditions of high temperature and high pressure. Thus, this process consumes a large amount of fossil fuels, and also brings great burden to the environment. The method of electrocatalytic nitrogen reduction (NRR) to synthesize ammonia has temporarily emerged. It synthesizes ammonia using nitrogen and water as raw materials under mild conditions of normal temperature and pressure, driven by sustainable energy sources such as solar and wind power, and can achieve the expected effects of green and zero emissions. However, it is found that the following three problems always exist in this process. First, the chemical property of nitrogen is stable, N≡N fracture requires a large energy. Second, in commonly used aqueous electrolytes, strong hydrogen evolution reaction (HER) tends to occur, resulting in lower selectivity for NRR. Third, due to the low solubility and slow diffusion of nitrogen in water, nitrogen supply at the reaction interface is always insufficient. Therefore, exploring and designing effective optimization schemes from the perspectives of electrocatalysts, electrolytes, and working electrodes for these three scientific issues is of great significance for further promoting the practical application of electrocatalytic nitrogen reduction reactions.
