4.7 Article

Thermodynamic feasibility analysis of distributed chemical looping ammonia synthesis

Journal

CHEMICAL ENGINEERING JOURNAL
Volume 426, Issue -, Pages -

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.131421

Keywords

Ammonia synthesis; Chemical looping; Process synthesis

Funding

  1. United Technologies Corporation Institute for Advanced Systems Engineering (UTC-IASE) of the University of Connecticut

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The paper explores intensified Chemical looping for Ammonia Synthesis (CLAS) as a process suitable for remote deployment at Stranded Natural Gas (SNG) sites, aiming to address the challenges in utilizing SNG. By systematically evaluating CLAS, promising chemical loops such as Ca3N2/CaH2, SrH2/Sr3N2, MnO2/Mn5N2 and MoO2/Mo2N are found, indicating potential for further research towards a distributed ammonia synthesis solution.
Stranded Natural Gas (SNG) flaring has increased over the last decade resulting in additional Green House Gas (GHG) emissions and underutilization of our finite fossil fuel resources. However, utilization of SNG is difficult due to its low volume, inconsistent composition, and intermittent flow. In this paper, intensified Chemical looping for Ammonia Synthesis (CLAS) is explored as a process suitable for remote deployment at SNG sites. CLAS mediate ammonia synthesis by using compounds that carry nitrogen and hydrogen in stepwise reactions, allowing ammonia synthesis under milder conditions and smaller, more flexible processes. The challenge in CLAS is to find a feasible combination of materials and process conditions that yield ammonia at economically acceptable rates. We propose a framework that systematically evaluates CLAS to determine their suitability for SNG deployment. CLAS reaction schemes are reviewed and organized based on the mediating compounds used to synthesize ammonia. Different compounds are evaluated for each CLAS in search of a thermodynamically spontaneous pair. Spontaneous CLAS flowsheets are, then, optimized to maximize ammonia output at equilibrium. The results are ranked against performance metrics of energy intensity, efficiency, and cost. Chemical loops with Ca3N2/CaH2, SrH2/Sr3N2, MnO2/Mn5N2 and MoO2/Mo2N are found to have favorable performance, along with literature-reported evidence and are recommended for further evaluation toward a distributed ammonia synthesis solution.

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