Home | << 1 >> |
![]() |
Records | |||||
---|---|---|---|---|---|
Author | Engelmann, Y.; Mehta, P.; Neyts, E.C.; Schneider, W.F.; Bogaerts, A. | ||||
Title | Predicted Influence of Plasma Activation on Nonoxidative Coupling of Methane on Transition Metal Catalysts | Type | A1 Journal article | ||
Year | 2020 | Publication | Acs Sustainable Chemistry & Engineering | Abbreviated Journal | Acs Sustain Chem Eng |
Volume | 8 | Issue | 15 | Pages | 6043-6054 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Movement Antwerp (MOVANT) | ||||
Abstract | The combination of catalysis and nonthermal plasma holds promise for enabling difficult chemical conversions. The possible synergy between both depends strongly on the nature of the reactive plasma species and the catalyst material. In this paper, we show how vibrationally excited species and plasma-generated radicals interact with transition metal catalysts and how changing the catalyst material can improve the conversion rates and product selectivity. We developed a microkinetic model to investigate the impact of vibrational excitations and plasma-generated radicals on the nonoxidative coupling of methane over transition metal surfaces. We predict a significant increase in ethylene formation for vibrationally excited methane. Plasma-generated radicals have a stronger impact on the turnover frequencies with high selectivity toward ethylene on noble catalysts and mixed selectivity on non-noble catalysts. In general, we show how the optimal catalyst material depends on the desired products as well as the plasma conditions. | ||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000526884000025 | Publication Date | 2020-04-20 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2168-0485 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.4 | Times cited | Open Access | ||
Notes | Herculesstichting; University of Notre Dame; Universiteit Antwerpen; Division of Engineering Education and Centers, EEC-1647722 ; We would like to thank Tom Butterworth for his work on methane vibrational distribution functions (VDF) and for sharing his thoughts and experiences on this matter, specifically regarding the VDF of the degenerate modes of methane. We ACS Sustainable Chemistry & Engineering pubs.acs.org/journal/ascecg Research Article https://dx.doi.org/10.1021/acssuschemeng.0c00906 ACS Sustainable Chem. Eng. 2020, 8, 6043−6054 6052 also acknowledge financial support from the DOC-PRO3 and the TOP-BOF projects of the University of Antwerp. This work was carried out in part using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen, a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (Department EWI), and the University of Antwerp. Support for W.F.S. was provided by the National Science Foundation under cooperative agreement no. EEC-1647722, an Engineering Research Center for the Innovative and Strategic Transformation of Alkane Resources (CISTAR). P.M. acknowledges support through the Eilers Graduate Fellowship of the University of Notre Dame. | Approved | Most recent IF: 8.4; 2020 IF: 5.951 | ||
Call Number | PLASMANT @ plasmant @c:irua:169228 | Serial | 6366 | ||
Permanent link to this record | |||||
Author | Vervloessem, E.; Aghaei, M.; Jardali, F.; Hafezkhiabani, N.; Bogaerts, A. | ||||
Title | Plasma-Based N2Fixation into NOx: Insights from Modeling toward Optimum Yields and Energy Costs in a Gliding Arc Plasmatron | Type | A1 Journal article | ||
Year | 2020 | Publication | Acs Sustainable Chemistry & Engineering | Abbreviated Journal | Acs Sustain Chem Eng |
Volume | 8 | Issue | 26 | Pages | 9711-9720 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Plasma technology provides a sustainable, fossil-free method for N2 fixation, i.e., the conversion of inert atmospheric N2 into valuable substances, such as NOx or ammonia. In this work, we present a novel gliding arc plasmatron at atmospheric pressure for NOx production at different N2/O2 gas feed ratios, offering a promising NOx yield of 1.5% with an energy cost of 3.6 MJ/mol NOx produced. To explain the underlying mechanisms, we present a chemical kinetics model, validated by experiments, which provides insight into the NOx formation pathways and into the ambivalent role of the vibrational kinetics. This allows us to pinpoint the factors limiting the yield and energy cost, which can help to further improve the process. | ||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000548456600013 | Publication Date | 2020-07-06 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2168-0485 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.4 | Times cited | Open Access | OpenAccess | |
Notes | Herculesstichting; Universiteit Antwerpen; Vlaamse regering; H2020 European Research Council, 810182 ; N2 Applied; Excellence of Science FWO – FNRS project, 30505023 GoF9618n ; | Approved | Most recent IF: 8.4; 2020 IF: 5.951 | ||
Call Number | PLASMANT @ plasmant @c:irua:170138 | Serial | 6392 | ||
Permanent link to this record | |||||
Author | Engelmann, Y.; van ’t Veer, K.; Gorbanev, Y.; Neyts, E.C.; Schneider, W.F.; Bogaerts, A. | ||||
Title | Plasma Catalysis for Ammonia Synthesis: A Microkinetic Modeling Study on the Contributions of Eley–Rideal Reactions | Type | A1 Journal Article;Plasma catalysis | ||
Year | 2021 | Publication | Acs Sustainable Chemistry & Engineering | Abbreviated Journal | Acs Sustain Chem Eng |
Volume | 9 | Issue | 39 | Pages | 13151-13163 |
Keywords | A1 Journal Article;Plasma catalysis; Eley−Rideal reactions; Volcano plots; Vibrational excitation; Radical reactions; Dielectric barrier discharge; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; | ||||
Abstract | Plasma catalysis is an emerging new technology for the electrification and downscaling of NH3 synthesis. Increasing attention is being paid to the optimization of plasma catalysis with respect to the plasma conditions, the catalyst material, and their mutual interaction. In this work we use microkinetic models to study how the total conversion process is impacted by the combination of different plasma conditions and transition metal catalysts. We study how plasma-generated radicals and vibrationally excited N2 (present in a dielectric barrier discharge plasma) interact with the catalyst and impact the NH3 turnover frequencies (TOFs). Both filamentary and uniform plasmas are studied, based on plasma chemistry models that provided plasma phase speciation and vibrational distribution functions. The Langmuir−Hinshelwood reaction rate coefficients (i.e., adsorption reactions and subsequent reactions among adsorbates) are determined using conventional scaling relations. An additional set of Eley−Rideal reactions (i.e., direct reactions of plasma radicals with adsorbates) was added and a sensitivity analysis on the assumed reaction rate coefficients was performed. We first show the impact of different vibrational distribution functions on the catalytic dissociation of N2 and subsequent production of NH3, and we gradually include more radical reactions, to illustrate the contribution of these species and their corresponding reaction pathways. Analysis over a large range of catalysts indicates that different transition metals (metals such as Rh, Ni, Pt, and Pd) optimize the NH3TOFs depending on the population of the vibrational levels of N2. At higher concentrations of plasma-generated radicals, the NH3 TOFs become less dependent on the catalyst material, due to radical adsorptions on the more noble catalysts and Eley−Rideal reactions on the less noble catalysts. | ||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000705367800004 | Publication Date | 2021-10-04 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2168-0485 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 5.951 | Times cited | Open Access | OpenAccess | |
Notes | Basic Energy Sciences, DE-SC0021107 ; Vlaamse regering, HBC.2019.0108 ; H2020 European Research Council, 810182 ; Methusalem project – University of Antwerp; Excellence of science FWO-FNRS, GoF9618n ; TOP-BOF – University of Antwerp; DOCPRO3 – University of Antwerp; We acknowledge the financial support from the DOC-PRO3, the TOP-BOF, and the Methusalem project of the University of Antwerp, as well as from the European Research Council (ERC) (grant agreement No, 810182−SCOPE ERC Synergy project), under the European Union’s Horizon 2020 research and innovation programme, the Flemish Government through the Moonshot cSBO project P2C (HBC.2019.0108), and the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023). Calculations were carried out using the Turing HPC infrastructure at the CalcUA core facility of the Universiteit Antwerpen, a division of the Flemish Supercomputer Center VSC, funded by the Hercules Foundation, the Flemish Government (Department EWI), 13162 | Approved | Most recent IF: 5.951 | ||
Call Number | PLASMANT @ plasmant @c:irua:182482 | Serial | 6811 | ||
Permanent link to this record | |||||
Author | Zhang, Y.; Qin, S.; Claes, N.; Schilling, W.; Sahoo, P.K.; Ching, H.Y.V.; Jaworski, A.; Lemière, F.; Slabon, A.; Van Doorslaer, S.; Bals, S.; Das, S. | ||||
Title | Direct Solar Energy-Mediated Synthesis of Tertiary Benzylic Alcohols Using a Metal-Free Heterogeneous Photocatalyst | Type | A1 Journal article | ||
Year | 2022 | Publication | ACS Sustainable Chemistry and Engineering | Abbreviated Journal | Acs Sustain Chem Eng |
Volume | 10 | Issue | 1 | Pages | 530-540 |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Organic synthesis (ORSY) | ||||
Abstract | Direct hydroxylation via the functionalization of tertiary benzylic C(sp3)-H bond is of great significance for obtaining tertiary alcohols which find wide applications in pharmaceuticals as well as in fine chemical industries. However, current synthetic procedures use toxic reagents and therefore, the development of a sustainable strategy for the synthesis of tertiary benzyl alcohols is highly desirable. To solve this problem, herein, we report a metal-free heterogeneous photocatalyst to synthesize the hydroxylated products using oxygen as the key reagent. Various benzylic substrates were employed into our mild reaction conditions to afford the desirable products in good to excellent yields. More importantly, gram-scale reaction was achieved via harvesting direct solar energy and exhibited high quantity of the product. The high stability of the catalyst was proved via recycling the catalyst and spectroscopic analyses. Finally, a possible mechanism was proposed based on the EPR and other experimental evidence. |
||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000736518000001 | Publication Date | 2022-01-10 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2168-0485 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.4 | Times cited | 24 | Open Access | OpenAccess |
Notes | We thank BOF joint PhD grant (to Y. Z.), Francqui Foundation and FWO research grant (to S.D.), Chinese Scholarship Council (to Y.Z.). A.S. would like to thank the Swedish Energy Agency for financial support (project nr: 5050-1). The SEM microscope was partly funded by the Hercules Fund from the Flemish Government. | Approved | Most recent IF: 8.4 | ||
Call Number | EMAT @ emat @c:irua:184744 | Serial | 6900 | ||
Permanent link to this record | |||||
Author | Queralto, A.; Graf, D.; Frohnhoven, R.; Fischer, T.; Vanrompay, H.; Bals, S.; Bartasyte, A.; Mathur, S. | ||||
Title | LaFeO3 nanofibers for high detection of sulfur-containing gases | Type | A1 Journal article | ||
Year | 2019 | Publication | ACS Sustainable Chemistry and Engineering | Abbreviated Journal | Acs Sustain Chem Eng |
Volume | 7 | Issue | 7 | Pages | 6023-6032 |
Keywords | A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) | ||||
Abstract | Lanthanum ferrite nanofibers were electrospun from a chemical sol and calcined at 600 degrees C to obtain singlephase LaFeO3 (LFO) perovskite. High-resolution transmission electron microscopy in conjunction with 3D tomographic analysis confirmed an interwoven network of hollow and porous (surface) LFO nanofibers. Owing to their high surface area and p-type behavior, the nanofiber meshes showed high chemoselectivity toward reducing toxic gases (SO2, H2S) that could be reproducibly detected at very low concentrations (<1 ppm), well below the threshold values for occupational safety and health. An increased sensitivity was observed in the temperature range of 150-300 degrees C with maximum sensor response at 250 degrees C. The surface reaction at the heterogeneous solid (LFO)/gas (SO2) interface that confirmed the formation of La-2(SO4)(3) was investigated by X-ray photoelectron spectroscopy. Moreover, the LFO fibers showed a high selectivity in the detection of oxidizing and reducing gases. Whereas superior detection of NH3 and H2S was measured, little response was observed for CO and NO2. Finally, the integration of nanowire meshes in commercial sensor platforms was successfully demonstrated. | ||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000461978200047 | Publication Date | 2019-02-21 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2168-0485 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 5.951 | Times cited | 41 | Open Access | OpenAccess |
Notes | ; The authors kindly acknowledge the ERA.Net RUS Plus project FONSENS funded by the German Federal Ministry of Education and Research (BMBF) under the grant no. 01DJ16017. A.Q. highly appreciates the support of the Alexander von Humboldt Foundation (grant no. AVH 1184642) and the BMBF for his postdoctoral fellowship. A.Q., D.G., R.F., T.F., and S.M. also kindly acknowledge the financial support of the University of Cologne. H.V. acknowledges financial support by the Research Foundation Flanders (FWO grant 1S32617N). S.B. acknowledges financial support from European Research Council (ERC Starting Grant #335078-COLOURATOMS). We also express our gratitude to Prof. Dr. J. Hadermann from the Electron Microscopy for Materials Science group at the University of Antwerp for her assistance. A.B. is grateful for the EUR EIPHI program (grant no. ANR-17-EURE-0002). ; | Approved | Most recent IF: 5.951 | ||
Call Number | UA @ admin @ c:irua:158535 | Serial | 5263 | ||
Permanent link to this record | |||||
Author | Gorbanev, Y.; Vervloessem, E.; Nikiforov, A.; Bogaerts, A. | ||||
Title | Nitrogen fixation with water vapor by nonequilibrium plasma : toward sustainable ammonia production | Type | A1 Journal article | ||
Year | 2020 | Publication | Acs Sustainable Chemistry & Engineering | Abbreviated Journal | Acs Sustain Chem Eng |
Volume | 8 | Issue | 7 | Pages | 2996-3004 |
Keywords | A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) | ||||
Abstract | Ammonia is a crucial nutrient used for plant growth and as a building block in the pharmaceutical and chemical industry, produced via nitrogen fixation of the ubiquitous atmospheric N2. Current industrial ammonia production relies heavily on fossil resources, but a lot of work is put into developing nonfossil-based pathways. Among these is the use of nonequilibrium plasma. In this work, we investigated water vapor as a H source for nitrogen fixation into NH3 by nonequilibrium plasma. The highest selectivity toward NH3 was observed with low amounts of added H2O vapor, but the highest production rate was reached at high H2O vapor contents. We also studied the role of H2O vapor and of the plasma-exposed liquid H2O in nitrogen fixation by using isotopically labeled water to distinguish between these two sources of H2O. We show that added H2O vapor, and not liquid H2O, is the main source of H for NH3 generation. The studied catalyst- and H2-free method offers excellent selectivity toward NH3 (up to 96%), with energy consumption (ca. 95–118 MJ/mol) in the range of many plasma-catalytic H2-utilizing processes. | ||||
Address | |||||
Corporate Author | Thesis | ||||
Publisher | Place of Publication | Editor | |||
Language | Wos | 000516665500045 | Publication Date | 2020-02-03 | |
Series Editor | Series Title | Abbreviated Series Title | |||
Series Volume | Series Issue | Edition | |||
ISSN | 2168-0485 | ISBN | Additional Links | UA library record; WoS full record; WoS citing articles | |
Impact Factor | 8.4 | Times cited | 14 | Open Access | |
Notes | ; This research was supported by the Excellence of Science FWO-FNRS project (FWO grant ID GoF9618n, EOS ID 30505023), the Catalisti Moonshot project P2C, and the Methusalem project of the University of Antwerp. ; | Approved | Most recent IF: 8.4; 2020 IF: 5.951 | ||
Call Number | UA @ admin @ c:irua:167134 | Serial | 6568 | ||
Permanent link to this record |