Research progress in electrochemical synthesis of ammonia catalysts

Recently, the research team of Zeng Jie, a professor at the University of Science and Technology of China, and Si Rui, a professor at the Shanghai Institute of Applied Physics, the Chinese Academy of Sciences, have collaborated to build an atomically dispersed ruthenium catalyst to achieve highly efficient nitrogen electroreduction to ammonia. The ammonia production rate of this ruthenium single-atom catalyst in the electrocatalytic reduction of nitrogen reaction is the highest value reported so far. The result was published in the "Advanced Materials" magazine (Adv. Mater. 2018, 30, 1803498), and was selected as the first illustration. The co-first authors of the paper are Geng Zhigang, a special associate researcher at the University of Science and Technology of China and Liu Yan, a doctoral student.

At present, high temperature and high pressure (150-350 atm, 350-550 ℃) are required for the industrial synthesis of ammonia by the Haber process. This demanding condition consumes 1-2% of the world's energy supply every year. In addition, the traditional Hubble method for ammonia synthesis requires hydrogen as one of the raw materials, and the traditional hydrogen production process will emit a large amount of CO2. Therefore, it is particularly important to explore the catalytic reaction of ammonia synthesis under mild conditions. The electrochemical reduction of ammonia to ammonia synthesis can be carried out at normal temperature and pressure, and water can be selected as the source of hydrogen, which has attracted wide attention from scientists. However, to date, the reported ammonia production rate of the electrocatalyst in the electrochemical reduction of nitrogen is very low, and it is difficult to meet the industrial needs. Therefore, it is a very challenging task to develop electrocatalysts that can efficiently electrochemically reduce nitrogen to ammonia.

To solve this problem, the researchers chose the metal-organic framework (ZIF-8) as the matrix, and added ruthenium-based compounds to the reaction precursors to control the form of ruthenium in the metal-organic framework. The researchers found that when less ruthenium-based compounds are added, a highly dispersed nitrogen-coordinated ruthenium single-atom catalyst (Ru SAs / NC) can be obtained. After increasing the input of ruthenium-based compounds, ruthenium will be dispersed in the form of small particles in the metal organic framework (Ru NPs / NC). Subsequently, the researchers applied these two catalysts to the electrochemical reduction of nitrogen, and found that the Ru SAs / NC catalyst can efficiently electrocatalyze the reduction of nitrogen to ammonia at a voltage of -0.2V relative to the standard hydrogen electrode. -1cat.h-1, the ammonia production rate is 1.98 times that of Ru NPs / NC. Experimental and theoretical calculations further reveal that the high-efficiency catalytic performance of the nitrogen-coordinated ruthenium monoatomic catalyst mainly comes from the efficient dissociation of the monoatomic catalyst to nitrogen molecules. This research work not only opened up a new way for single-atom catalysts in the electrochemical synthesis of ammonia, but also further promoted the possibility of electrochemical synthesis of ammonia in practical applications.

This research was supported by the National Academy of Sciences Key Frontier Science Research Project, the Ministry of Science and Technology, the National Natural Science Foundation of China, and Anhui Province Key Research and Development Program.

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