Dielectric barrier discharge plasma-assisted catalytic ammonia synthesis:synergistic effect of Ni-MOF-74 catalyst and nanosecond pulsed plasma

Ammonia is one of the most important chemical raw materials in both manufacture and life of human.Traditionally Haber-Bosch method for ammonia synthesis involves high temperature and high pressure conditions,leading to significant energy consumption and environmental pollution.Non-thermal plasma(NTP) is a promising alternative approach to ammonia synthesis at low temperature and atmospheric pressure.In this study,the synergistic effect of nanosecond pulsed dielectric barrier discharge(np-DBD) and Ni-MOF-74 catalyst was investigated in ammonia synthesis by utilizing nitrogen and hydrogen as feedstock.The results demonstrated that the plasma catalytic-synthesis process parameters play a crucial role in the synthesis process of ammonia.The highest ammonia synthesis rate of 5145.16 μmol·g^(-1)·h^(-1)with an energy efficiency of 1.27 g·kWh^(-1)was observed in the presence of the Ni-MOF-74 catalyst,which was3.7 times higher than that without Ni-MOF-74 catalyst.The synergistic effect of Ni-MOF-74catalyst and nanosecond pulsed plasma was explored by in-situ plasma discharge diagnostics.

Effects of O_(2) addition on the plasma uniformity and reactivity of Ar DBD excited by ns pulsed and AC power supplies

Dielectric barrier discharges(DBDs)have been widely used in ozone synthesis,materials surface treatment,and plasma medicine for their advantages of uniform discharge and high plasmachemical reactivity.To improve the reactivity of DBDs,in this work,the O_(2) is added into Ar nanosecond(ns)pulsed and AC DBDs.The uniformity and discharge characteristics of Ar ns pulsed and AC DBDs with different O_(2) contents are investigated with optical and electrical diagnosis methods.The DBD uniformity is quantitatively analyzed by gray value standard deviation method.The electrical parameters are extracted from voltage and current waveforms separation to characterize the discharge processes and calculate electron density n_(e).The optical emission spectroscopy is measured to show the plasma reactivity and calculate the trend of electron temperature T_(e) with the ratio of two emission lines.It is found that the ns pulsed DBD has a much better uniformity than AC DBD for the fast rising and falling time.With the addition of O_(2),the uniformity of ns pulsed DBD gets worse for the space electric field distortion by O_(2)^(-),which promotes the filamentary formation.While,in AC DBD,the added O_(2) can reduce the intensity of filaments,which enhances the discharge uniformity.The ns pulsed DBD has a much higher instantaneous power and energy efficiency than AC DBD.The ratio of Ar emission intensities indicates that the T_(e) drops quickly with the addition of O_(2) both ns pulsed and AC DBDs and the ns pulsed DBD has an obvious higher T_(e) and n_(e) than AC DBD.The results are helpful for the realization of the reactive and uniform low temperature plasma sources.