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Author |
Meng, S.; Li, S.; Sun, S.; Bogaerts, A.; Liu, Y.; Yi, Y. |
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Title |
NH3 decomposition for H2 production by thermal and plasma catalysis using bimetallic catalysts |
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A1 Journal Article |
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Year  |
2024 |
Publication |
Chemical Engineering Science |
Abbreviated Journal |
Chemical Engineering Science |
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Volume |
283 |
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Pages |
119449 |
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Keywords |
A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
Plasma catalysis has emerged as a promising approach for driving thermodynamically unfavorable chemical
reactions. Nevertheless, comprehending the mechanisms involved remains a challenge, leading to uncertainty
about whether the optimal catalyst in plasma catalysis aligns with that in thermal catalysis. In this research, we
explore this question by studying monometallic catalysts (Fe, Co, Ni and Mo) and bimetallic catalysts (Fe-Co, Mo-
Co, Fe-Ni and Mo-Ni) in both thermal catalytic and plasma catalytic NH3 decomposition. Our findings reveal that
the Fe-Co bimetallic catalyst exhibits the highest activity in thermal catalysis, the Fe-Ni bimetallic catalyst
outperforms others in plasma catalysis, indicating a discrepancy between the optimal catalysts for the two
catalytic modes in NH3 decomposition. Comprehensive catalyst characterization, kinetic analysis, temperature
program surface reaction experiments and plasma diagnosis are employed to discuss the key factors influencing
NH3 decomposition performance. |
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Wos |
001105312500001 |
Publication Date |
2023-10-28 |
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Edition |
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ISSN |
0009-2509 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
4.7 |
Times cited |
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Open Access |
Not_Open_Access |
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Notes |
Universiteit Antwerpen, 32249 ; National Natural Science Foundation of China, 21503032 ; PetroChina Innovation Foundation, 2018D-5007-0501 ; |
Approved |
Most recent IF: 4.7; 2024 IF: 2.895 |
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Call Number |
PLASMANT @ plasmant @c:irua:201009 |
Serial |
8967 |
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Author |
Andersen, Ja.; van 't Veer, K.; Christensen, Jm.; Østberg, M.; Bogaerts, A.; Jensen, Ad. |
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Title |
Ammonia decomposition in a dielectric barrier discharge plasma: Insights from experiments and kinetic modeling |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Chemical engineering science |
Abbreviated Journal |
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Volume |
271 |
Issue |
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Pages |
118550 |
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Keywords |
A1 Journal article; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
Utilizing ammonia as a storage medium for hydrogen is currently receiving increased attention. A possible method to retrieve the hydrogen is by plasma-catalytic decomposition. In this work, we combined an experimental study, using a dielectric barrier discharge plasma reactor, with a plasma kinetic model, to get insights into the decomposition mechanism. The experimental results revealed a similar effect on the ammonia conversion when changing the flow rate and power, where increasing the specific energy input (higher power or lower flow rate) gave an increased conversion. A conversion as high as 82 % was achieved at a specific energy input of 18 kJ/Nl. Furthermore, when changing the discharge volume from 31 to 10 cm3, a change in the plasma distribution factor from 0.2 to 0.1 was needed in the model to best describe the conversions of the experiments. This means that a smaller plasma volume caused a higher transfer of energy through micro-discharges (non-uniform plasma), which was found to promote the decomposition of ammonia. These results indicate that it is the collisions between NH3 and the high-energy electrons that initiate the decomposition. Moreover, the rate of ammonia destruction was found by the model to be in the order of 1022 molecules/(cm3 s) during the micro-discharges, which is 5 to 6 orders of magnitude higher than in the afterglows. A considerable re-formation of ammonia was found to take place in the afterglows, limiting the overall conversion. In addition, the model revealed that implementation of packing material in the plasma introduced high concentrations of surface-bound hydrogen atoms, which introduced an additional ammonia re-formation pathway through an Eley-Rideal reaction with gas phase NH2. Furthermore, a more uniform plasma is predicted in the presence of MgAl2O4, which leads to a lower average electron energy during micro-discharges and a lower conversion (37 %) at a comparable residence time for the plasma alone (51 %). |
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000946293200001 |
Publication Date |
2023-02-09 |
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ISSN |
0009-2509 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.7 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
We thank Topsoe A/S for providing the packing material used, the research group PLASMANT (UAntwerpen) for sharing their plasma kinetic model and allowing us to perform the calculations on their clusters, and the Department of Chemical and Biochemical Engineering, Technical University of Denmark, for funding this project. |
Approved |
Most recent IF: 4.7; 2023 IF: 2.895 |
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Call Number |
PLASMANT @ plasmant @c:irua:195204 |
Serial |
7237 |
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Author |
Peng, L.; Kassotaki, E.; Liu, Y.; Sun, J.; Dai, X.; Pijuan, M.; Rodriguez-Roda, I.; Buttiglieri, G.; Ni, B.-J. |
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Title |
Modelling cometabolic biotransformation of sulfamethoxazole by an enriched ammonia oxidizing bacteria culture |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Chemical engineering science |
Abbreviated Journal |
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Volume |
173 |
Issue |
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Pages |
465-473 |
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Keywords |
A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
Antibiotics such as sulfamethoxazole (SFX) are environmentally hazardous after being released into the aquatic environment and challenges remain in the development of engineered prevention strategies. In this work, a mathematical model was developed to describe and evaluate cometabolic biotransformation of SFX and its transformation products (TPs) in an enriched ammonia oxidizing bacteria (AOB) culture. The growth-linked cometabolic biodegradation by AOB, non-growth transformation by AOB and nongrowth transformation by heterotrophs were considered in the model framework. The production of major TPs comprising 4-Nitro-SFX, Desamino-SFX and N-4-Acetyl-SFX was also specifically modelled. The validity of the model was demonstrated through testing against literature reported data from extensive batch tests, as well as from long-term experiments in a partial nitritation sequencing batch reactor (SBR) and in a combined SBR + membrane aerated biofilm reactor performing nitrification/denitrification. Modelling results revealed that the removal efficiency of SFX increased with the increase of influent ammonium concentration, whereas the influent organic matter, hydraulic retention time and solid retention time exerted a limited effect on SFX biodegradation with the removal efficiencies varying in a narrow range. The variation of influent SFX concentration had no impact on SFX removal efficiency. The established model framework enables interpretation of a range of experimental observations on SFX biodegradation and helps to identify the optimal conditions for efficient removal. (C) 2017 Elsevier Ltd. All rights reserved. |
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000411764200039 |
Publication Date |
2017-08-14 |
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ISSN |
0009-2509 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Open Access |
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Notes |
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Approved |
no |
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Call Number |
UA @ admin @ c:irua:146629 |
Serial |
8267 |
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Author |
Liu, Y.; Ngo, H.H.; Guo, W.; Zhou, J.; Peng, L.; Wang, D.; Chen, X.; Sun, J.; Ni, B.-J. |
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Title |
Optimizing sulfur-driven mixotrophic denitrification process : system performance and nitrous oxide emission |
Type |
A1 Journal article |
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Year |
2017 |
Publication |
Chemical engineering science |
Abbreviated Journal |
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Volume |
172 |
Issue |
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Pages |
414-422 |
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Keywords |
A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
Nitrate contamination of groundwater has been recognized as a significant environmental problem world widely. Sulfur-driven mixotrophic denitrification has been demonstrated as a promising groundwater treatment process, which though plays an important role in nitrous oxide (N2O) emissions, significantly contributing to the overall carbon footprint of the system. However, the current process optimizations only focus on nitrate removal and excess sulfate control, with the N2O emission being ignored. In this work, an integrated mathematical model was proposed to evaluate the N2O emission as well as the excess sulfate production and carbon source utilization in sulfur-driven mixotrophic denitrification process. In this model, autotrophic and heterotrophic denitrifiers use their corresponding electron donors (sulfur and organic matter, respectively) to reduce nitrate to nitrogen gas, with each modeled as three-step denitrification (NO3 to N-2 via NO2 and N2O) driven by sulfur or organic matter to describe all potential N2O accumulation steps. The developed model, employing model parameters previously reported in literature, was successfully validated using N2O and sulfate data from two mixotrophic denitrification systems with different initial conditions. Modeling results revealed substantial N2O accumulation due to the relatively low autotrophic N2O reduction activity as compared to heterotrophic N2O reduction activity, explaining the observation that higher carbon source addition resulted in lower N2O accumulation in sulfur-driven mixotrophic denitrifying system. Based on the validated model, optimizations of the overall system performance were carried out. Application of the model to simulate long-term operations of sulfur-driven mixotrophic denitrification process indicates that longer sludge retention time reduces N2O emission due to better retention of active biomass. High-level total nitrogen removal with significant N2O emission mitigation, appropriate excess sulfate control and maximized COD utilization can be achieved simultaneously through controlling the influent nitrate and COD concentrations. (C) 2017 Elsevier Ltd. All rights reserved. |
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000410833900034 |
Publication Date |
2017-07-03 |
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0009-2509 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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no |
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Call Number |
UA @ admin @ c:irua:146634 |
Serial |
8344 |
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