CC3 porous organic cage crystals and membranes for the non-thermal plasma catalytic ammonia synthesis
Ammonia is considered a basic building block for fertilizers. Also, it is an economically efficient and technologically suitable solution for energy storage and transportation. Non-thermal plasma-driven catalysis powered by renewable energy is considered as a green alternative to the conventional Ha...
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| Format: | Article |
| Language: | English |
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Elsevier
2022-08-01
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| Series: | Chemical Engineering Journal Advances |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S2666821122001004 |
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| author | Fnu Gorky Hoang M. Nguyen Jolie M. Lucero Shelby Guthrie James M. Crawford Moises A. Carreon Maria L. Carreon |
| author_facet | Fnu Gorky Hoang M. Nguyen Jolie M. Lucero Shelby Guthrie James M. Crawford Moises A. Carreon Maria L. Carreon |
| author_sort | Fnu Gorky |
| collection | DOAJ |
| description | Ammonia is considered a basic building block for fertilizers. Also, it is an economically efficient and technologically suitable solution for energy storage and transportation. Non-thermal plasma-driven catalysis powered by renewable energy is considered as a green alternative to the conventional Haber-Bosch process for ammonia synthesis. The main challenge in this electron-mediated route is the low ammonia synthesis production, given the plasma-induced decomposition of the freshly generated ammonia during the reaction. Herein we report the plasma-assisted ammonia synthesis in a dielectric barrier discharge reactor packed with CC3 crystals, a prototypical porous organic cage, and a molecular-sieve membrane fabricated from the same CC3 material. The CC3 crystals delivered the highest ammonia synthesis rate (0.06 μmol min−1 m−2) compared to other microporous catalysts such as zeolite (SAPO-34) and metal-organic frameworks (ZIF-8, ZIF-67) (below 0.02 μmol min−1 m−2). The CC3 porous cage with well-defined octahedral crystal geometry provides partial protection while the CC3 membrane offers both adsorption and separation effects for the freshly formed ammonia from its in-situ decomposition, securing an excellent ammonia synthesis rate of 20.3 μmol min−1 m−2. The findings from this work unfolds novel insights into rational designs of advanced porous catalyst and membrane for plasma-driven catalytic ammonia synthesis in a sustainable and efficient way. |
| first_indexed | 2024-12-11T18:30:14Z |
| format | Article |
| id | doaj.art-f91d5489796641c3bc9ca3beab8d1dc3 |
| institution | Directory Open Access Journal |
| issn | 2666-8211 |
| language | English |
| last_indexed | 2024-12-11T18:30:14Z |
| publishDate | 2022-08-01 |
| publisher | Elsevier |
| record_format | Article |
| series | Chemical Engineering Journal Advances |
| spelling | doaj.art-f91d5489796641c3bc9ca3beab8d1dc32022-12-22T00:54:56ZengElsevierChemical Engineering Journal Advances2666-82112022-08-0111100340CC3 porous organic cage crystals and membranes for the non-thermal plasma catalytic ammonia synthesisFnu Gorky0Hoang M. Nguyen1Jolie M. Lucero2Shelby Guthrie3James M. Crawford4Moises A. Carreon5Maria L. Carreon6Chemical and Biological Engineering Department, South Dakota School of Mines & Technology, 501 E Saint Joseph St, Rapid City, SD, 57701, USAMechanical Engineering Department, University of Massachusetts Lowell, Lowell, MA, 01854, USAChemical and Biological Engineering Department, Colorado School of Mines, Golden, CO, 80401, USAChemical and Biological Engineering Department, South Dakota School of Mines & Technology, 501 E Saint Joseph St, Rapid City, SD, 57701, USAChemical and Biological Engineering Department, Colorado School of Mines, Golden, CO, 80401, USAChemical and Biological Engineering Department, Colorado School of Mines, Golden, CO, 80401, USA; Corresponding authors.Mechanical Engineering Department, University of Massachusetts Lowell, Lowell, MA, 01854, USA; Corresponding authors.Ammonia is considered a basic building block for fertilizers. Also, it is an economically efficient and technologically suitable solution for energy storage and transportation. Non-thermal plasma-driven catalysis powered by renewable energy is considered as a green alternative to the conventional Haber-Bosch process for ammonia synthesis. The main challenge in this electron-mediated route is the low ammonia synthesis production, given the plasma-induced decomposition of the freshly generated ammonia during the reaction. Herein we report the plasma-assisted ammonia synthesis in a dielectric barrier discharge reactor packed with CC3 crystals, a prototypical porous organic cage, and a molecular-sieve membrane fabricated from the same CC3 material. The CC3 crystals delivered the highest ammonia synthesis rate (0.06 μmol min−1 m−2) compared to other microporous catalysts such as zeolite (SAPO-34) and metal-organic frameworks (ZIF-8, ZIF-67) (below 0.02 μmol min−1 m−2). The CC3 porous cage with well-defined octahedral crystal geometry provides partial protection while the CC3 membrane offers both adsorption and separation effects for the freshly formed ammonia from its in-situ decomposition, securing an excellent ammonia synthesis rate of 20.3 μmol min−1 m−2. The findings from this work unfolds novel insights into rational designs of advanced porous catalyst and membrane for plasma-driven catalytic ammonia synthesis in a sustainable and efficient way.http://www.sciencedirect.com/science/article/pii/S2666821122001004Non-thermal plasmaPlasma catalysisAmmonia synthesisPorous organic cagesAdvanced porous catalystMembranes |
| spellingShingle | Fnu Gorky Hoang M. Nguyen Jolie M. Lucero Shelby Guthrie James M. Crawford Moises A. Carreon Maria L. Carreon CC3 porous organic cage crystals and membranes for the non-thermal plasma catalytic ammonia synthesis Chemical Engineering Journal Advances Non-thermal plasma Plasma catalysis Ammonia synthesis Porous organic cages Advanced porous catalyst Membranes |
| title | CC3 porous organic cage crystals and membranes for the non-thermal plasma catalytic ammonia synthesis |
| title_full | CC3 porous organic cage crystals and membranes for the non-thermal plasma catalytic ammonia synthesis |
| title_fullStr | CC3 porous organic cage crystals and membranes for the non-thermal plasma catalytic ammonia synthesis |
| title_full_unstemmed | CC3 porous organic cage crystals and membranes for the non-thermal plasma catalytic ammonia synthesis |
| title_short | CC3 porous organic cage crystals and membranes for the non-thermal plasma catalytic ammonia synthesis |
| title_sort | cc3 porous organic cage crystals and membranes for the non thermal plasma catalytic ammonia synthesis |
| topic | Non-thermal plasma Plasma catalysis Ammonia synthesis Porous organic cages Advanced porous catalyst Membranes |
| url | http://www.sciencedirect.com/science/article/pii/S2666821122001004 |
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