Two-Step Chemical Looping Cycle for Renewable NH3 Production Based on Non-Catalytic Co3Mo3N/Co6Mo6N Reactions

Nguyen, Nhu Pailes; Kaur, Shaspreet; Bush, H. Evan; Miller, James E.; Ambrosini, Andrea; Loutzenhiser, Peter G.

doi:10.1002/aenm.202302740

Two-Step Chemical Looping Cycle for Renewable NH₃ Production Based on Non-Catalytic Co₃Mo₃N/Co₆Mo₆N Reactions

Journal Article · Sun Dec 10 23:00:00 EST 2023 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202302740· OSTI ID:2333738

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Georgia Institute of Technology, Atlanta, GA (United States)
Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)
Arizona State Univ., Tempe, AZ (United States)

A two-step solar thermochemical looping cycle based on Co₃Mo₃N/Co₆Mo₆N reduction/nitridation reactions offers a pathway for green NH₃ production that utilizes concentrated solar irradiation, H₂O, and air as feedstocks. The NH₃ production cycle steps both derive process heat from concentrated solar irradiation and encompass 1) the reduction of Co₃Mo₃N in H₂ to Co₆Mo₆N and NH₃; and 2) nitridation of Co₆Mo₆N to Co₃Mo₃N with N₂. Co₃Mo₃N reduction/nitridation reactions are examined at different H₂ and/or N₂ partial pressures and temperatures. NH₃ production is quantified in situ using liquid conductivity measurements coupled with mass spectrometry (MS). Solid-state characterization is performed to identify a surface oxygen layer that necessitates the addition of H₂ during cycling to prevent surface oxidation by trace amounts of O₂. H₂ concentrations of > 5% H₂/Ar and temperatures >500 °C are required to reduce Co₃Mo₃N to Co₆Mo₆N and form NH₃ at 1 bar. Complete regeneration of Co₃Mo₃N from Co₆Mo₆N is achieved at conditions of 700 °C under 25–75% H₂/N₂. H₂ pressure-swings are observed to increase NH₃ production during Co₃Mo₃N reduction. In conclusion, the results represent the first comprehensive characterization of and definitive non-catalytic production of NH₃ via chemical looping with metal nitrides and provide insights for technology development.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office

Grant/Contract Number:: NA0003525

OSTI ID:: 2333738

Report Number(s):: SAND--2024-03978J

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 7 Vol. 14; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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