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      Plasma-enhanced catalytic synthesis of ammonia over a Ni/Al2O3 catalyst at near-room temperature: Insights into the importance of the catalyst surface on the reaction mechanism

      , , , , , ,
      ACS Catalysis
      American Chemical Society (ACS)

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          Abstract

          A better fundamental understanding of the plasma-catalyst interaction and the reaction mechanism is vital for optimizing the design of catalysts for ammonia synthesis by plasma-catalysis. In this work, we report on a hybrid plasma-enhanced catalytic process for the synthesis of ammonia directly from N2 and H2 over transition metal catalysts (M/Al2O3, M = Fe, Ni, Cu) at near room temperature (∼35 °C) and atmospheric pressure. Reactions were conducted in a specially designed coaxial dielectric barrier discharge (DBD) plasma reactor using water as a ground electrode, which could cool and maintain the reaction at near-room temperature. The transparency of the water electrode enabled operando optical diagnostics (intensified charge-coupled device (ICCD) imaging and optical emission spectroscopy) of the full plasma discharge area to be conducted without altering the operation of the reactor, as is often needed when using coaxial reactors with opaque ground electrodes. Compared to plasma synthesis of NH3 without a catalyst, plasma-catalysis significantly enhanced the NH3 synthesis rate and energy efficiency. The effect of different transition metal catalysts on the physical properties of the discharge is negligible, which suggests that the catalytic effects provided by the chemistry of the catalyst surface are dominant over the physical effects of the catalysts in the plasma-catalytic synthesis of ammonia. The highest NH3 synthesis rate of 471 μmol g–1 h–1 was achieved using Ni/Al2O3 as a catalyst with plasma, which is 100% higher than that obtained using plasma only. The presence of a transition metal (e.g., Ni) on the surface of Al2O3 provided a more uniform plasma discharge than Al2O3 or plasma only, and enhanced the mean electron energy. The mechanism of plasma-catalytic ammonia synthesis has been investigated through operando plasma diagnostics combined with comprehensive characterization of the catalysts using N2 physisorption measurements, X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), NH3-temperature-programmed desorption (TPD), and N2-TPD. Four forms of adsorbed NH x (x = 0, 1, 2, and 3) species were detected on the surfaces of the spent catalysts using XPS. It was found that metal sites and weak acid sites could enhance the production of NH3 via formation of NH2 intermediates on the surface.

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              Ammonia synthesis at atmospheric pressure

              Ammonia was synthesized from its elements at atmospheric pressure in a solid state proton (H+)-conducting cell-reactor. Hydrogen was flowing over the anode and was converted into protons that were transported through the solid electrolyte and reached the cathode (palladium) over which nitrogen was passing. At 570 degreesC and atmospheric pressure, greater than 78 percent of the electrochemically supplied hydrogen was converted into ammonia. The thermodynamic requirement for a high-pressure process is eliminated.
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                Author and article information

                Journal
                ACS Catalysis
                ACS Catal.
                American Chemical Society (ACS)
                2155-5435
                2155-5435
                October 18 2019
                October 18 2019
                Article
                10.1021/acscatal.9b02538
                3b155a8e-e359-45e8-b8b5-8fd1d5381cbf
                © 2019
                History

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