Plasma (catalyst) assisted nitrogen fixation reactor development for nitric oxide and ammonia production
This chapter focuses on the production of NOx from air and air+O2 is investigated in a pulsed powered milli scale gliding arc (GA) reactor, aiming at a containerized process for fertilizer production. First, the electrical parameters of the gliding arc reactor, such as frequency, pulse width, and amplitude of input voltage are investigated. Influence of process parameters such as feed mixture, flowrate, feed preheating, and effect of Ar and O2 content in feed are also investigated at varying specific energy input. The findings are correlated with high speed imaging of the GA dynamics. Increase in frequency, pulse width and input voltage amplitude resulted in an increased specific energy input, which lead to increase in NOx production. An O2 content of 40 48% was optimum, with an enhancement of ~20% in NOx production. Addition of Ar and preheating of the feed resulted in lower NOx production. 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Anastasopoulou, S. Butala, B. S. Patil, J. Lang, V. Hessel, Q. Wang, Submitt. to Process. 2016. CHAPTER 2 PLASMA ASSISTED NITROGEN OXIDE PRODUCTION FROM AIR IN A GLIDING ARC REACTOR: CHARACTERIZATION FOR ELECTRICAL AND PROCESS PARAMETERS This chapter has been adapted from: Patil, B. S. F. J. J. Peeters, Medrano J. A. Gerard van Rooij, Gallucci F. Lang, J. Wang, Q. Hessel, V. (2016) Plasma nitrogen oxide production from air at atmospheric pressure using a pulse powered milli scale gliding arc reactor. Submitted to AIChEJ. Patil, B. S. Rovira Palau, Joan, Hessel, V. Lang, J. Wang, Q. (2016) Plasma nitrogen oxides synthesis in a milli scale gliding arc reactor: investigating the electrical and process parameters. Plasma Chem. Plasma Proc. 36(1) 241 257. Abstract This chapter focuses on the production of NOx from air and air+O2 is investigated in a pulsed powered milli scale gliding arc (GA) reactor, aiming at a containerized process for fertilizer production. First, the electrical parameters of the gliding arc reactor, such as frequency, pulse width, and amplitude of input voltage are investigated. Influence of process parameters such as feed mixture, flowrate, feed preheating, and effect of Ar and O2 content in feed are also investigated at varying specific energy input. The findings are correlated with high speed imaging of the GA dynamics. Increase in frequency, pulse width and input voltage amplitude resulted in an increased specific energy input, which lead to increase in NOx production. An O2 content of 40 48% was optimum, with an enhancement of ~20% in NOx production. Addition of Ar and preheating of the feed resulted in lower NOx production. The volume covered by GA depends strongly on the gas flowrate, emphasizing that the gas flowrate has a major impact on the GA dynamics and the reaction kinetics. For 0.5 L/min, 1.4 vol% of NOx concentration was realized.This chapter focuses on the production of NOx from air and air+O2 is investigated in a pulsed powered milli scale gliding arc (GA) reactor, aiming at a containerized process for fertilizer production. First, the electrical parameters of the gliding arc reactor, such as frequency, pulse width, and amplitude of input voltage are investigated. Influence of process parameters such as feed mixture, flowrate, feed preheating, and effect of Ar and O2 content in feed are also investigated at varying specific energy input. The findings are correlated with high speed imaging of the GA dynamics. Increase in frequency, pulse width and input voltage amplitude resulted in an increased specific energy input, which lead to increase in NOx production. An O2 content of 40 48% was optimum, with an enhancement of ~20% in NOx production. Addition of Ar and preheating of the feed resulted in lower NOx production. The volume covered by GA depends strongly on the gas flowrate, emphasizing that the gas flowrate has a major impact on the GA dynamics and the reaction kinetics. For 0.5 L/min, 1.4 vol% of NOx concentration was realized. 2 Chapter 2 NOx Production in Milli scale Gliding Arc Reactor Page 22 2.1 Introduction Among several alternatives, electricity driven non equilibrium plasma processes are considered to be very attractive contenders for energy efficient nitrogen fixation[9,10] It is worth noting that nitrogen fixation via nonthermal plasma (NTP) offers an opportunity to produce fossil free nitrogen oxides due its 3.5 times lower theoretical energy requirement[11,12] In NTP, highly energetic electrons collide with bulk gas molecules, yielding a mixture of highly reactive species which enable thermodynamically unfavorable reactions like nitrogen fixation at low temperatures and atmospheric pressures[13,14] Plasma processes are more attractive on smaller scales like in containers or modular plants[15] Plasma assisted nitrogen fixation offers an interesting opportunity as atmospheric pressure and ambient temperature processing will substantially improve plant safety and decrease the operational and capital costs compared to the high pressure HaberBosch process[16] The mild operating conditions and relatively small scale could also encourage development of localized nitrogen fertilizer production plants. The approach of decentralized chemical production has been undertaken in the EU funded MAPSYN project for plasma assisted nitrogen fixation process[11,12] which would eventually benefit remote places to produce their own fertilizer and fuels, using only renewable energy sources such as solar or wind[17] along similar lines, N2 applied, a Norwegian company, is commercializing the plasma assisted nitrogen fixation process on smaller scale for use by farmers[18] The overall reactions representing nitrogen fixation with oxygen to give NOx (NO NO2) which further absorbed in water to yield nitric acid are depicted by reaction R1 and R2. The ratio of NO and NO2 is determined by thermodynamic equilibrium and the reaction kinetics[29] The reaction enthalpy of the process (DH) is fairly high, therefore high energy is needed to carry out this reaction. DHf= 90.4 kJ mol 1 (R1) DHf= 33.2 kJ mol