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A special issue of Catalysts (ISSN 2073-4344). This special issue belongs to the section "Environmental Catalysis".

Deadline for manuscript submissions: closed (30 November 2018) | Viewed by 73113

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Prof. Dr. Annemie Bogaerts

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Department of Chemistry, University of Antwerp, Campus Drie Eiken – Room B2.09, Universiteitsplein 1, Wilrijk, BE-2610 Antwerp, Belgium
Interests: plasma and plasma–surface interactions by means of computer modeling and experiments, for various applications, with a major focus on green chemistry; plasma catalysis
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Dear Colleagues,

Plasma catalysis is gaining increasing interest for various gas conversion applications, such as CO₂ conversion into value-added chemicals and fuels, N₂ fixation for the synthesis of NH₃ or NO_x, methane conversion into higher hydrocarbons or oxygenates. It is also widely used for air pollution control (e.g., VOC remediation). Plasma catalysis allows thermodynamically difficult reactions to proceed at ambient pressure and temperature, due to activation of the gas molecules by energetic electrons created in the plasma. However, plasma is very reactive but not selective, and thus a catalyst is needed to improve the selectivity.

In spite of the growing interest in plasma catalysis, the underlying mechanisms of the (possible) synergy between plasma and catalyst are not yet fully understood. Indeed, plasma catalysis is quite complicated, as the plasma will affect the catalyst and vice versa. Moreover, due to the reactive plasma environment, the most suitable catalysts will probably be different from thermal catalysts. More research is needed to better understand the plasma–catalyst interactions, in order to further improve the applications.

Submissions to this Special Issue are welcome in the form of original research papers or short reviews that reflect the state of the art in the above-mentioned applications.

Prof. Dr. Annemie Bogaerts
Guest Editor

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Keywords

Plasma–catalyst interaction
CO₂ conversion
N₂ fixation
CH₄ conversion
Air pollution control
Plasma catalysis synergy
Plasma reactor
Dielectric barrier discharge
Ambient conditions

Published Papers (13 papers)

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Editorial

Jump to: Research, Review

5 pages, 184 KiB

Open AccessEditorial

Editorial Catalysts: Special Issue on Plasma Catalysis

by Annemie Bogaerts

Catalysts 2019, 9(2), 196; https://doi.org/10.3390/catal9020196 - 21 Feb 2019

Cited by 6 | Viewed by 3858

Abstract

(This article belongs to the Special Issue Plasma Catalysis)

Research

Jump to: Editorial, Review

25 pages, 15013 KiB

Open AccessArticle

Plasma Catalysis: Distinguishing between Thermal and Chemical Effects

by Guido Giammaria, Gerard van Rooij and Leon Lefferts

Catalysts 2019, 9(2), 185; https://doi.org/10.3390/catal9020185 - 16 Feb 2019

Cited by 20 | Viewed by 5104

Abstract

The goal of this study is to develop a method to distinguish between plasma chemistry and thermal effects in a Dielectric Barrier Discharge nonequilibrium plasma containing a packed bed of porous particles. Decomposition of CaCO₃ in Ar plasma is used as a model reaction and CaCO₃ samples were prepared with different external surface area, via the particle size, as well as with different internal surface area, via pore morphology. Also, the effect of the CO₂ in gas phase on the formation of products during plasma enhanced decomposition is measured. The internal surface area is not exposed to plasma and relates to thermal effect only, whereas both plasma and thermal effects occur at the external surface area. Decomposition rates were in our case found to be influenced by internal surface changes only and thermal decomposition is concluded to dominate. This is further supported by the slow response in the CO₂ concentration at a timescale of typically 1 minute upon changes in discharge power. The thermal effect is estimated based on the kinetics of the CaCO₃ decomposition, resulting in a temperature increase within 80 °C for plasma power from 0 to 6 W. In contrast, CO₂ dissociation to CO and O₂ is controlled by plasma chemistry as this reaction is thermodynamically impossible without plasma, in agreement with fast response within a few seconds of the CO concentration when changing plasma power. CO forms exclusively via consecutive dissociation of CO₂ in the gas phase and not directly from CaCO₃. In ongoing work, this methodology is used to distinguish between thermal effects and plasma–chemical effects in more reactive plasma, containing, e.g., H₂. Full article

(This article belongs to the Special Issue Plasma Catalysis)

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13 pages, 4868 KiB

Open AccessCommunication

Highly Dispersed Co Nanoparticles Prepared by an Improved Method for Plasma-Driven NH₃ Decomposition to Produce H₂

by Li Wang, YanHui Yi, HongChen Guo, XiaoMin Du, Bin Zhu and YiMin Zhu

Catalysts 2019, 9(2), 107; https://doi.org/10.3390/catal9020107 - 22 Jan 2019

Cited by 29 | Viewed by 3902

Abstract

Previous studies reveal that combining non-thermal plasma with cheap metal catalysts achieved a significant synergy of enhancing performance of NH₃ decomposition, and this synergy strongly depended on the properties of the catalyst used. In this study, techniques of vacuum-freeze drying and plasma calcination were employed to improve the conventional preparation method of catalyst, aiming to enhance the activity of plasma-catalytic NH₃ decomposition. Compared with the activity of the catalyst prepared by a conventional method, the conversion of NH₃ significantly increased by 47% when Co/fumed SiO₂ was prepared by the improved method, and the energy efficiency of H₂ production increased from 2.3 to 5.7 mol(kW·h)⁻¹ as well. So far, the highest energy efficiency of H₂ formation of 15.9 mol(kW·h)⁻¹ was achieved on improved prepared Co/fumed SiO₂ with 98.0% ammonia conversion at the optimal conditions. The improved preparation method enables cobalt species to be highly dispersed on fumed SiO₂ support, which creates more active sites. Besides, interaction of Co with fumed SiO₂ and acidity of the catalyst were strengthened according to results of H₂-TPR and NH₃-probe experiments, respectively. These results demonstrate that employing vacuum-freeze drying and plasma calcination during catalyst preparation is an effective approach to manipulate the properties of catalyst, and enables the catalyst to display high activity towards plasma-catalytic NH₃ decomposition to produce H₂. Full article

(This article belongs to the Special Issue Plasma Catalysis)

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22 pages, 11296 KiB

Open AccessArticle

High-Efficiency Catalytic Conversion of NO_x by the Synergy of Nanocatalyst and Plasma: Effect of Mn-Based Bimetallic Active Species

by Yan Gao, Wenchao Jiang, Tao Luan, Hui Li, Wenke Zhang, Wenchen Feng and Haolin Jiang

Catalysts 2019, 9(1), 103; https://doi.org/10.3390/catal9010103 - 18 Jan 2019

Cited by 18 | Viewed by 4746

Abstract

Three typical Mn-based bimetallic nanocatalysts of Mn−Fe/TiO₂, Mn−Co/TiO₂, Mn−Ce/TiO₂ were synthesized via the hydrothermal method to reveal the synergistic effects of dielectric barrier discharge (DBD) plasma and bimetallic nanocatalysts on NO_x catalytic conversion. The plasma-catalyst hybrid catalysis was investigated compared with the catalytic effects of plasma alone and nanocatalyst alone. During the catalytic process of catalyst alone, the catalytic activities of all tested catalysts were lower than 20% at ambient temperature. While in the plasma-catalyst hybrid catalytic process, NO_x conversion significantly improved with discharge energy enlarging. The maximum NO_x conversion of about 99.5% achieved over Mn−Ce/TiO₂ under discharge energy of 15 W·h/m³ at ambient temperature. The reaction temperature had an inhibiting effect on plasma-catalyst hybrid catalysis. Among these three Mn-based bimetallic nanocatalysts, Mn−Ce/TiO₂ displayed the optimal catalytic property with higher catalytic activity and superior selectivity in the plasma-catalyst hybrid catalytic process. Furthermore, the physicochemical properties of these three typical Mn-based bimetallic nanocatalysts were analyzed by N₂ adsorption, Transmission Electron Microscope (TEM), X-ray diffraction (XRD), H₂-temperature-programmed reduction (TPR), NH₃-temperature-programmed desorption (TPD), and X-ray photoelectron spectroscopy (XPS). The multiple characterizations demonstrated that the plasma-catalyst hybrid catalytic performance was highly dependent on the phase compositions. Mn−Ce/TiO₂ nanocatalyst presented the optimal structure characteristic among all tested samples, with the largest surface area, the minished particle sizes, the reduced crystallinity, and the increased active components distributions. In the meantime, the ratios of Mn⁴⁺/(Mn²⁺ + Mn³⁺ + Mn⁴⁺) in the Mn−Ce/TiO₂ sample was the highest, which was beneficial to plasma-catalyst hybrid catalysis. Generally, it was verified that the plasma-catalyst hybrid catalytic process with the Mn-based bimetallic nanocatalysts was an effective approach for high-efficiency catalytic conversion of NO_x, especially at ambient temperature. Full article

(This article belongs to the Special Issue Plasma Catalysis)

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32 pages, 3915 KiB

Open AccessArticle

Altering Conversion and Product Selectivity of Dry Reforming of Methane in a Dielectric Barrier Discharge by Changing the Dielectric Packing Material

by Inne Michielsen, Yannick Uytdenhouwen, Annemie Bogaerts and Vera Meynen

Catalysts 2019, 9(1), 51; https://doi.org/10.3390/catal9010051 - 07 Jan 2019

Cited by 40 | Viewed by 5052 | Correction

Abstract

We studied the influence of dense, spherical packing materials, with different chemical compositions, on the dry reforming of methane (DRM) in a dielectric barrier discharge (DBD) reactor. Although not catalytically activated, a vast effect on the conversion and product selectivity could already be observed, an influence which is often neglected when catalytically activated plasma packing materials are being studied. The α-Al₂O₃ packing material of 2.0–2.24 mm size yields the highest total conversion (28%), as well as CO₂ (23%) and CH₄ (33%) conversion and a high product fraction towards CO (~70%) and ethane (~14%), together with an enhanced CO/H₂ ratio of 9 in a 4.5 mm gap DBD at 60 W and 23 kHz. γ-Al₂O₃ is only slightly less active in total conversion (22%) but is even more selective in products formed than α-Al₂O₃. BaTiO₃ produces substantially more oxygenated products than the other packing materials but is the least selective in product fractions and has a clear negative impact on CO₂ conversion upon addition of CH₄. Interestingly, when comparing to pure CO₂ splitting and when evaluating differences in products formed, significantly different trends are obtained for the packing materials, indicating a complex impact of the presence of CH₄ and the specific nature of the packing materials on the DRM process. Full article

(This article belongs to the Special Issue Plasma Catalysis)

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12 pages, 1267 KiB

Open AccessArticle

Isotope Labelling for Reaction Mechanism Analysis in DBD Plasma Processes

by Paula Navascués, Jose M. Obrero-Pérez, José Cotrino, Agustín R. González-Elipe and Ana Gómez-Ramírez

Catalysts 2019, 9(1), 45; https://doi.org/10.3390/catal9010045 - 04 Jan 2019

Cited by 14 | Viewed by 3685

Abstract

Dielectric barrier discharge (DBD) plasmas and plasma catalysis are becoming an alternative procedure to activate various gas phase reactions. A low-temperature and normal operating pressure are the main advantages of these processes, but a limited energy efficiency and little selectivity control hinder their practical implementation. In this work, we propose the use of isotope labelling to retrieve information about the intermediate reactions that may intervene during the DBD processes contributing to a decrease in their energy efficiency. The results are shown for the wet reforming reaction of methane, using D₂O instead of H₂O as reactant, and for the ammonia synthesis, using NH₃/D₂/N₂ mixtures. In the two cases, it was found that a significant amount of outlet gas molecules, either reactants or products, have deuterium in their structure (e.g., HD for hydrogen, CD_xH_y for methane, or ND_xH_y for ammonia). From the analysis of the evolution of the labelled molecules as a function of power, useful information has been obtained about the exchange events of H by D atoms (or vice versa) between the plasma intermediate species. An evaluation of the number of these events revealed a significant progression with the plasma power, a tendency that is recognized to be detrimental for the energy efficiency of reactant to product transformation. The labelling technique is proposed as a useful approach for the analysis of plasma reaction mechanisms. Full article

(This article belongs to the Special Issue Plasma Catalysis)

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20 pages, 9155 KiB

Open AccessFeature PaperArticle

Destruction of Toluene, Naphthalene and Phenanthrene as Model Tar Compounds in a Modified Rotating Gliding Arc Discharge Reactor

by Xiangzhi Kong, Hao Zhang, Xiaodong Li, Ruiyang Xu, Ishrat Mubeen, Li Li and Jianhua Yan

Catalysts 2019, 9(1), 19; https://doi.org/10.3390/catal9010019 - 28 Dec 2018

Cited by 20 | Viewed by 4420

Abstract

Tar removal is one of the greatest technical challenges of commercial gasification technologies. To find an efficient way to destroy tar with plasma, a rotating gliding arc (RGA) discharge reactor equipped with a fan-shaped swirling generator was used for model tar destruction in this study. The solution of toluene, naphthalene and phenanthrene is used as a tar surrogate and is destroyed in humid nitrogen. The influence of tar, CO₂ and moisture concentrations, and the discharge current on the destruction efficiency is emphasized. In addition, the combination of Ni/γ-Al₂O₃ catalyst with plasma was tested for plasma catalytic tar destruction. The toluene, naphthalene and phenanthrene destruction efficiency reached up to 95.2%, 88.9%, and 83.9% respectively, with a content of 12 g/Nm³ tar, 12% moisture, 15% CO_2, and a flow rate of 6 NL/min, whereas 9.3 g/kW·h energy efficiency was achieved. The increase of discharge current is advantageous in terms of decreasing black carbon production. The participation of Ni/γ-Al₂O₃ catalyst shows considerable improvement in destruction efficiency, especially at a relatively high flow rate (over 9 NL/min). The major liquid by-products are phenylethyne, indene, acenaphthylene and fluoranthene. The first two are majorly converted from toluene, acenaphthylene is produced by the co-reaction of toluene and naphthalene in the plasma, and fluoranthene is converted by phenanthrene. Full article

(This article belongs to the Special Issue Plasma Catalysis)

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10 pages, 1428 KiB

Open AccessArticle

Ammonia Plasma-Catalytic Synthesis Using Low Melting Point Alloys

by Javishk R. Shah, Joshua M. Harrison and Maria L. Carreon

Catalysts 2018, 8(10), 437; https://doi.org/10.3390/catal8100437 - 03 Oct 2018

Cited by 32 | Viewed by 6225

Abstract

The Haber-Bosch process has been the commercial benchmark process for ammonia synthesis for more than a century. Plasma-catalytic synthesis for ammonia production is theorized to have a great potential for being a greener alternative to the Haber-Bosch process. However, the underlying reactions for ammonia synthesis still require some detailed study especially for radiofrequency plasmas. Herein, the use of inductively coupled radiofrequency plasma for the synthesis of ammonia when employing Ga, In and their alloys as catalysts is presented. The plasma is characterized using emission spectroscopy and the surface of catalysts using Scanning Electron Microscope. A maximum energy yield of 0.31 g-NH₃/kWh and energy cost of 196 MJ/mol is achieved with Ga-In (0.6:0.4 and 0.2:0.8) alloy at 50 W plasma power. Granular nodes are observed on the surface of catalysts indicating the formation of the intermediate GaN. Full article

(This article belongs to the Special Issue Plasma Catalysis)

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13 pages, 1894 KiB

Open AccessArticle

Plasma Oxidation of H₂S over Non-stoichiometric La_xMnO₃ Perovskite Catalysts in a Dielectric Barrier Discharge Reactor

by Kejie Xuan, Xinbo Zhu, Yuxiang Cai and Xin Tu

Catalysts 2018, 8(8), 317; https://doi.org/10.3390/catal8080317 - 02 Aug 2018

Cited by 21 | Viewed by 4523

Abstract

In this work, plasma-catalytic removal of H₂S over La_xMnO₃ (x = 0.90, 0.95, 1, 1.05 and 1.10) has been studied in a coaxial dielectric barrier discharge (DBD) reactor. The non-stoichiometric effect of the La_xMnO₃ catalysts on the removal of H₂S and sulfur balance in the plasma-catalytic process has been investigated as a function of specific energy density (SED). The integration of the plasma with the La_xMnO₃ catalysts significantly enhanced the reaction performance compared to the process using plasma alone. The highest H₂S removal of 96.4% and sulfur balance of 90.5% were achieved over the La_0.90MnO₃ catalyst, while the major products included SO₂ and SO₃. The missing sulfur could be ascribed to the sulfur deposited on the catalyst surfaces. The non-stoichiometric La_xMnO₃ catalyst exhibited larger specific surface areas and smaller crystallite sizes compared to the LaMnO₃ catalyst. The non-stoichiometric effect changed their redox properties as the decreased La/Mn ratio favored the transformation of Mn³⁺ to Mn⁴⁺, which contributed to the generation of oxygen vacancies on the catalyst surfaces. The XPS and H₂-TPR results confirmed that the Mn-rich catalysts showed the higher relative concentration of surface adsorbed oxygen (O_ads) and lower reduction temperature compared to LaMnO₃ catalyst. The reaction performance of the plasma-catalytic oxidation of H₂S is closely related to the relative concentration of O_ads formed on the catalyst surfaces and the reducibility of the catalysts. Full article

(This article belongs to the Special Issue Plasma Catalysis)

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15 pages, 1871 KiB

Open AccessArticle

Plasma-Catalytic Mineralization of Toluene Adsorbed on CeO₂

by Zixian Jia, Xianjie Wang, Emeric Foucher, Frederic Thevenet and Antoine Rousseau

Catalysts 2018, 8(8), 303; https://doi.org/10.3390/catal8080303 - 27 Jul 2018

Cited by 11 | Viewed by 3961

Abstract

In the context of coupling nonthermal plasmas with catalytic materials, CeO₂ is used as adsorbent for toluene and combined with plasma for toluene oxidation. Two configurations are addressed for the regeneration of toluene saturated CeO₂: (i) in plasma-catalysis (IPC); and (ii) post plasma-catalysis (PPC). As an advanced oxidation technique, the performances of toluene mineralization by the plasma-catalytic systems are evaluated and compared through the formation of CO₂. First, the adsorption of 100 ppm of toluene onto CeO₂ is characterized in detail. Total, reversible and irreversible adsorbed fractions are quantified. Specific attention is paid to the influence of relative humidity (RH): (i) on the adsorption of toluene on CeO₂; and (ii) on the formation of ozone in IPC and PPC reactors. Then, the mineralization yield and the mineralization efficiency of adsorbed toluene are defined and investigated as a function of the specific input energy (SIE). Under these conditions, IPC and PPC reactors are compared. Interestingly, the highest mineralization yield and efficiency are achieved using the in-situ configuration operated with the lowest SIE, that is, lean conditions of ozone. Based on these results, the specific impact of RH on the IPC treatment of toluene adsorbed on CeO₂ is addressed. Taking into account the impact of RH on toluene adsorption and ozone production, it is evidenced that the mineralization of toluene adsorbed on CeO₂ is directly controlled by the amount of ozone produced by the discharge and decomposed on the surface of the coupling material. Results highlight the key role of ozone in the mineralization process and the possible detrimental effect of moisture. Full article

(This article belongs to the Special Issue Plasma Catalysis)

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11 pages, 3151 KiB

Open AccessArticle

DBD Plasma-ZrO₂ Catalytic Decomposition of CO₂ at Low Temperatures

by Amin Zhou, Dong Chen, Cunhua Ma, Feng Yu and Bin Dai

Catalysts 2018, 8(7), 256; https://doi.org/10.3390/catal8070256 - 23 Jun 2018

Cited by 41 | Viewed by 5325

Abstract

This study describes the decomposition of CO₂ using Dielectric Barrier Discharge (DBD) plasma technology combined with the packing materials. A self-cooling coaxial cylinder DBD reactor that packed ZrO₂ pellets or glass beads with a grain size of 1–2 mm was designed to decompose CO₂. The control of the temperature of the reactor was achieved via passing the condensate water through the shell of the DBD reactor. Key factors, for instance discharge length, packing materials, beads size and discharge power, were investigated to evaluate the efficiency of CO₂ decomposition. The results indicated that packing materials exhibited a prominent effect on CO₂ decomposition, especially in the presence of ZrO₂ pellets. Most encouragingly, a maximum decomposition rate of 49.1% (2-mm particle sizes) and 52.1% (1-mm particle sizes) was obtained with packing ZrO₂ pellets and a 32.3% (2-mm particle sizes) and a 33.5% (1-mm particle sizes) decomposing rate with packing glass beads. In the meantime, CO selectivity was up to 95%. Furthermore, the energy efficiency was increased from 3.3%–7% before and after packing ZrO₂ pellets into the DBD reactor. It was concluded that the packing ZrO₂ simultaneously increases the key values, decomposition rate and energy efficiency, by a factor of two, which makes it very promising. The improved decomposition rate and energy efficiency can be attributed mainly to the stronger electric field and electron energy and the lower reaction temperature. Full article

(This article belongs to the Special Issue Plasma Catalysis)

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18 pages, 5364 KiB

Open AccessArticle

Mode Transition of Filaments in Packed-Bed Dielectric Barrier Discharges

by Mingxiang Gao, Ya Zhang, Hongyu Wang, Bin Guo, Quanzhi Zhang and Annemie Bogaerts

Catalysts 2018, 8(6), 248; https://doi.org/10.3390/catal8060248 - 15 Jun 2018

Cited by 22 | Viewed by 4472

Abstract

We investigated the mode transition from volume to surface discharge in a packed bed dielectric barrier discharge reactor by a two-dimensional particle-in-cell/Monte Carlo collision method. The calculations are performed at atmospheric pressure for various driving voltages and for gas mixtures with different N [...] Read more.

_{2}

and O

_{2}

compositions. Our results reveal that both a change of the driving voltage and gas mixture can induce mode transition. Upon increasing voltage, a mode transition from hybrid (volume+surface) discharge to pure surface discharge occurs, because the charged species can escape much more easily to the beads and charge the bead surface due to the strong electric field at high driving voltage. This significant surface charging will further enhance the tangential component of the electric field along the dielectric bead surface, yielding surface ionization waves (SIWs). The SIWs will give rise to a high concentration of reactive species on the surface, and thus possibly enhance the surface activity of the beads, which might be of interest for plasma catalysis. Indeed, electron impact excitation and ionization mainly take place near the bead surface. In addition, the propagation speed of SIWs becomes faster with increasing N

_{2}

content in the gas mixture, and slower with increasing O

_{2}

content, due to the loss of electrons by attachment to O

_{2}

molecules. Indeed, the negative O

_{2}^{-}

ion density produced by electron impact attachment is much higher than the electron and positive O

_{2}^{+}

ion density. The different ionization rates between N

_{2}

and O

_{2}

gases will create different amounts of electrons and ions on the dielectric bead surface, which might also have effects in plasma catalysis. Full article

(This article belongs to the Special Issue Plasma Catalysis)

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Review

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40 pages, 8134 KiB

Open AccessEditor’s ChoiceReview

The Use of Zeolites for VOCs Abatement by Combining Non-Thermal Plasma, Adsorption, and/or Catalysis: A Review

by Savita K. P. Veerapandian, Nathalie De Geyter, Jean-Marc Giraudon, Jean-François Lamonier and Rino Morent

Catalysts 2019, 9(1), 98; https://doi.org/10.3390/catal9010098 - 17 Jan 2019

Cited by 111 | Viewed by 14803

Abstract

Non-thermal plasma technique can be easily integrated with catalysis and adsorption for environmental applications such as volatile organic compound (VOC) abatement to overcome the shortcomings of individual techniques. This review attempts to give an overview of the literature about the application of zeolite as adsorbent and catalyst in combination with non-thermal plasma for VOC abatement in flue gas. The superior surface properties of zeolites in combination with its excellent catalytic properties obtained by metal loading make it an ideal packing material for adsorption plasma catalytic removal of VOCs. This work highlights the use of zeolites for cyclic adsorption plasma catalysis in order to reduce the energy cost to decompose per VOC molecule and to regenerate zeolites via plasma. Full article

(This article belongs to the Special Issue Plasma Catalysis)

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