Abstract <p>Ammonia (NH<sub>3</sub>) plays a crucial role in human life both as a critical chemical feedstock for fertilizers and as a potential renewable energy carrier. The Haber–Bosch process is the state of the art approach to synthesize ammonia which releases 1–1.5% of anthropogenic CO<sub>2</sub>. Chemical looping ammonia synthesis (CLAS) using nitride formation to activate nitrogen is an alternative to the Haber–Bosch approach and here the focus is on the kinetics of CLAS. Reaction order, reaction rate constant (<i>K</i>), and activation energy (<i>E</i><sub>a</sub>) at 550–800°C and atmospheric pressure were investigated. The order of reaction in nitrogen and hydrogen is estimated from 0.45 to 1.35, and 1.25 to 2.1 respectively. The optimum temperature to maximize the NH<sub>3</sub> production rate for CLAS using Mn at atmospheric pressure is estimated at 650°C. The possible mechanisms for CLAS based on Mn/Mn nitride at atmospheric pressure and elevated temperature are proposed here.</p>

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Chemical Looping of Manganese to Synthesize Ammonia at Atmospheric Pressure: Kinetics and Proposed Mechanism

  • Wrya Aframehr,
  • Peter H. Pfromm

摘要

Abstract

Ammonia (NH3) plays a crucial role in human life both as a critical chemical feedstock for fertilizers and as a potential renewable energy carrier. The Haber–Bosch process is the state of the art approach to synthesize ammonia which releases 1–1.5% of anthropogenic CO2. Chemical looping ammonia synthesis (CLAS) using nitride formation to activate nitrogen is an alternative to the Haber–Bosch approach and here the focus is on the kinetics of CLAS. Reaction order, reaction rate constant (K), and activation energy (Ea) at 550–800°C and atmospheric pressure were investigated. The order of reaction in nitrogen and hydrogen is estimated from 0.45 to 1.35, and 1.25 to 2.1 respectively. The optimum temperature to maximize the NH3 production rate for CLAS using Mn at atmospheric pressure is estimated at 650°C. The possible mechanisms for CLAS based on Mn/Mn nitride at atmospheric pressure and elevated temperature are proposed here.