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A Plasma-Water Droplet Reactor for Process-Intensified, Continuous Nitrogen Fixation at Atmospheric Pressure
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2020-09-04 , DOI: 10.1021/acssuschemeng.0c04432 Joseph R. Toth 1 , Nabiel H. Abuyazid 1 , Daniel J. Lacks 1 , Julie N. Renner 1 , R. Mohan Sankaran 1
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2020-09-04 , DOI: 10.1021/acssuschemeng.0c04432 Joseph R. Toth 1 , Nabiel H. Abuyazid 1 , Daniel J. Lacks 1 , Julie N. Renner 1 , R. Mohan Sankaran 1
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Current industrial production of ammonia via the Haber–Bosch process has a massive carbon footprint because the hydrogen gas feedstock comes from the reformation of fossil fuel which releases large amounts of carbon dioxide. One possible solution is to provide hydrogen gas by water electrolysis that is powered by renewable sources. A more radical solution is to use water as the hydrogen source in a process-intensified scheme whereby ammonia is produced by directly reacting nitrogen gas and water. Here, we investigated an atmospheric-pressure plasma process to continuously produce ammonia from nitrogen gas and atomized water droplets. The successful production of ammonia was carefully confirmed by several control experiments. We find that other forms of fixed nitrogen are synthesized as well, predominantly nitrate and some nitrite. To understand the role of water droplets, we characterized their lifetimes in the reactor and compared the ammonia production with a water vapor feed. The results show that the ammonia forms through gas-phase chemistry and the liquid phase does not appear to substantially contribute. Additional insight into the reaction mechanism was provided by replacing the water with hydrogen gas or oxygen gas as the feedstock. As expected, no nitrates or nitrites were synthesized with hydrogen gas, and the ammonia production was comparable, indicating similar mechanisms may be occurring that involve feedstock dissociation to atomic hydrogen. No ammonia or nitrates/nitrites were detected with oxygen gas, which suggests that water provides a unique reaction pathway for nitric and nitrous acid to be formed in the gas phase. Our study demonstrates that nitrogen gas and water droplets can serve as feeds in a plasma process for the sustainable and distributed production of ammonia or other fixed nitrogen compounds.
中文翻译：
等离子水滴反应器，用于在大气压下进行过程增强的连续固氮
当前通过哈伯-博世（Haber-Bosch）工艺进行的氨工业生产具有巨大的碳足迹，因为氢气原料来自化石燃料的重整，释放出大量的二氧化碳。一种可能的解决方案是通过由可再生资源提供动力的水电解来提供氢气。一种更彻底的解决方案是在过程增强方案中将水用作氢源，从而通过使氮气与水直接反应生成氨。在这里，我们研究了一种常压等离子体工艺，该工艺从氮气和雾化的水滴连续产生氨。几个对照实验仔细地证实了氨的成功生产。我们发现还合成了其他形式的固定氮，主要是硝酸盐和一些亚硝酸盐。为了了解水滴的作用，我们表征了水滴在反应器中的寿命，并将氨的产生与水蒸气进料进行了比较。结果表明，氨是通过气相化学反应形成的，而液相似乎基本上没有贡献。通过用氢气或氧气作为原料代替水，可以进一步了解反应机理。不出所料，没有硝酸盐或亚硝酸盐是与氢气合成的，氨的产生是可比的，这表明可能发生了类似的机理，其中涉及原料离解成原子氢。氧气未检测到氨或硝酸盐/亚硝酸盐，这表明水为气相中的硝酸和亚硝酸提供了独特的反应途径。
更新日期：2020-10-05
中文翻译：
等离子水滴反应器，用于在大气压下进行过程增强的连续固氮
当前通过哈伯-博世（Haber-Bosch）工艺进行的氨工业生产具有巨大的碳足迹，因为氢气原料来自化石燃料的重整，释放出大量的二氧化碳。一种可能的解决方案是通过由可再生资源提供动力的水电解来提供氢气。一种更彻底的解决方案是在过程增强方案中将水用作氢源，从而通过使氮气与水直接反应生成氨。在这里，我们研究了一种常压等离子体工艺，该工艺从氮气和雾化的水滴连续产生氨。几个对照实验仔细地证实了氨的成功生产。我们发现还合成了其他形式的固定氮，主要是硝酸盐和一些亚硝酸盐。为了了解水滴的作用，我们表征了水滴在反应器中的寿命，并将氨的产生与水蒸气进料进行了比较。结果表明，氨是通过气相化学反应形成的，而液相似乎基本上没有贡献。通过用氢气或氧气作为原料代替水，可以进一步了解反应机理。不出所料，没有硝酸盐或亚硝酸盐是与氢气合成的，氨的产生是可比的，这表明可能发生了类似的机理，其中涉及原料离解成原子氢。氧气未检测到氨或硝酸盐/亚硝酸盐，这表明水为气相中的硝酸和亚硝酸提供了独特的反应途径。
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