The direct oxidation of nitrogen is a potential pathway to achieving the zero-carbon-emission synthesis of nitric acid or nitrate, because it does not involve ammonia synthesis and additional ammonia oxidation process...The direct oxidation of nitrogen is a potential pathway to achieving the zero-carbon-emission synthesis of nitric acid or nitrate, because it does not involve ammonia synthesis and additional ammonia oxidation processes. However, the slow kinetics of nitrogen oxidation and the difficult selective control of oxidation products hinder the development of this process. In this study, a plasma-driven gas-liquid relay reaction system was developed to overcome these limitations. A typical feature of this reaction system is that it can efficiently generate NO_x under plasma exposure;moreover, the specific anions in the absorption solution can be oxidized to strong oxidants capable of relay oxidation of low-valence nitrogen oxides. This feature allows for the deep oxidation of nitrogen, thus enabling the oxidation products of nitrogen to exist in high-valence states in the absorption solution. For experimental verification, we achieved the 100% selective synthesis of nitrate under plasma exposure, with air as the supply gas and a sodium sulfate solution as the absorption solution.展开更多
基金supported by the National Key R&D Program of China (2021YFB4000402)the National Natural Science Foundation of China (22022503)。
文摘The direct oxidation of nitrogen is a potential pathway to achieving the zero-carbon-emission synthesis of nitric acid or nitrate, because it does not involve ammonia synthesis and additional ammonia oxidation processes. However, the slow kinetics of nitrogen oxidation and the difficult selective control of oxidation products hinder the development of this process. In this study, a plasma-driven gas-liquid relay reaction system was developed to overcome these limitations. A typical feature of this reaction system is that it can efficiently generate NO_x under plasma exposure;moreover, the specific anions in the absorption solution can be oxidized to strong oxidants capable of relay oxidation of low-valence nitrogen oxides. This feature allows for the deep oxidation of nitrogen, thus enabling the oxidation products of nitrogen to exist in high-valence states in the absorption solution. For experimental verification, we achieved the 100% selective synthesis of nitrate under plasma exposure, with air as the supply gas and a sodium sulfate solution as the absorption solution.
