TY - JOUR
T1 - Achieving +95% Ammonia Purity by Optimizing the Absorption and Desorption Conditions of Supported Metal Halides
AU - Hrtus, Daniel J.
AU - Nowrin, Fouzia Hasan
AU - Lomas, Austin
AU - Fotsa, Yanick
AU - Malmali, Mahdi
N1 - Funding Information:
This material is based upon work supported by the U.S. Department of Energy’s Office of Energy Efficiency and Renewable Energy (EERE) under the Solar Energy Technologies Office (SETO) Award Number DE-EE0009802. This paper describes objective technical results and analysis. Any subjective views or opinions that might be expressed in the paper do not necessarily represent the views of the U.S. Department of Energy or the United States Government.
Publisher Copyright:
© 2021 American Chemical Society.
PY - 2022/1/10
Y1 - 2022/1/10
N2 - The worldwide push toward the reduction of carbon dioxide emissions has been the main motivation for finding a sustainable alternative to the conventional Haber-Bosch ammonia production process that has a significant carbon footprint. In this work, we focused on ammonia separation by replacing the condenser with an absorber column packed with metal halide solid absorbents. These salts had shown promise in selective separation of NH3 in the past, but more information on the cyclic operation and ammonia desorption conditions was needed. We used an automated apparatus equipped with an absorption column packed with either silica, supported CaCl2, or supported MgCl2 to explore the optimal absorption/desorption conditions (pressure and temperature swings). Primarily, we are reporting on the working capacity of various sorbents for cyclic ammonia separation. Additionally, we investigated the effect of sweep gas on the desorption efficiency and compared the absorbent performance among each other in terms of absorption working capacity and the purity of the ammonia product stream. We were able to achieve an NH3 stream with a purity of over 95%; in some of the tests, we achieved a coordination number as high as 2.5 molNH3/molsalt, which is the highest ever reported for a dynamic flow breakthrough test. Our experiments further prove the significant potential that these salts possess to replace phase change condensation in the conventional ammonia synthesis-not only in a greener fashion but also more efficiently with a decreased equipment size, with reduced energy input in smaller scales, and with more flexibility to follow intermittent renewables.
AB - The worldwide push toward the reduction of carbon dioxide emissions has been the main motivation for finding a sustainable alternative to the conventional Haber-Bosch ammonia production process that has a significant carbon footprint. In this work, we focused on ammonia separation by replacing the condenser with an absorber column packed with metal halide solid absorbents. These salts had shown promise in selective separation of NH3 in the past, but more information on the cyclic operation and ammonia desorption conditions was needed. We used an automated apparatus equipped with an absorption column packed with either silica, supported CaCl2, or supported MgCl2 to explore the optimal absorption/desorption conditions (pressure and temperature swings). Primarily, we are reporting on the working capacity of various sorbents for cyclic ammonia separation. Additionally, we investigated the effect of sweep gas on the desorption efficiency and compared the absorbent performance among each other in terms of absorption working capacity and the purity of the ammonia product stream. We were able to achieve an NH3 stream with a purity of over 95%; in some of the tests, we achieved a coordination number as high as 2.5 molNH3/molsalt, which is the highest ever reported for a dynamic flow breakthrough test. Our experiments further prove the significant potential that these salts possess to replace phase change condensation in the conventional ammonia synthesis-not only in a greener fashion but also more efficiently with a decreased equipment size, with reduced energy input in smaller scales, and with more flexibility to follow intermittent renewables.
KW - absorption
KW - ammonia
KW - desorption
KW - distributed manufacturing
KW - metal halide
KW - purity
KW - support
UR - http://www.scopus.com/inward/record.url?scp=85121918824&partnerID=8YFLogxK
U2 - 10.1021/acssuschemeng.1c05668
DO - 10.1021/acssuschemeng.1c05668
M3 - Article
AN - SCOPUS:85121918824
VL - 10
SP - 204
EP - 212
JO - ACS Sustainable Chemistry and Engineering
JF - ACS Sustainable Chemistry and Engineering
SN - 2168-0485
IS - 1
ER -