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Catalysts
Special Issues
Heterogeneous Selective and Total Catalytic Oxidation
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Heterogeneous Selective and Total Catalytic Oxidation

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

Deadline for manuscript submissions: closed (30 April 2022) | Viewed by 34858

Special Issue Editors

Dr. Sabine Valange

E-Mail Website
Guest Editor
Institut de Chimie des Milieux et Matériaux de Poitiers (IC2MP), UMR CNRS 7285, Université de Poitiers, Ecole Nationale Supérieure d'Ingénieurs de Poitiers, 1 Rue Marcel Doré, TSA 41105, CEDEX 9, 86073 Poitiers, France
Interests: catalyst synthesis; porous materials; nanostructured oxides; heterogeneous catalysis; selective oxidation; total oxidation; biomass valorization; ball-milling; ultrasound; sonochemistry; sonocatalysis; sustainable chemistry
Special Issues, Collections and Topics in MDPI journals
Prof. Dr. Jacques Charles Védrine

E-Mail Website
Guest Editor
Laboratoire de Réactivité de Surface, Faculté des Sciences et Ingénierie, Sorbonne Université, UMR-CNRS 7197, 4 Place Jussieu, F-75252 Paris, France
Interests: heterogeneous catalysis (acid–base and selective oxidation reactions); physical techniques of characterization; metal oxide catalysts; zeolites and porous materials; heterpolyoxometallates
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Heterogeneous catalytic oxidation is a vital key enabling technology for the production of value-added organic chemicals, as well as for depollution/remediation purposes. Most industrial processes involve selective (partial) and total oxidation reactions in either gas or liquid phase. For instance, the selective oxidation of alcohols to carbonyl compounds (e.g., aldehydes, ketones, carboxylic acids, esters) is a key domain for industry, as well as those reactions leading to olefins from alkanes or aldehydes, carboxylic acids, and nitriles from olefins or alkanes. The abatement of organic pollutants for clean air or water purification/treatment also covers a large part of the heterogeneous catalytic oxidation reactions. This includes atmospheric pollutants such as volatile organic compounds (VOCs), NH3, CO, CH4, etc., and a variety of organic pollutants in liquid phase, such as dyes, phenols, pesticides, pharmaceuticals, and personal care products.

Selective and total catalytic oxidation reactions offer many advantages, but there is still a need for catalysts with improved performance. In both cases, the control of the selectivity to the desired product is the major challenge to be overcome. Additionally, with the increased environmental issues and legislation constraints, energy-efficient heterogeneous catalytic oxidation processes have to be promoted for a more sustainable world. In this respect, physical activation methods based on, for instance, ultrasound and microwave irradiations, ball milling (reactive grinding), non-thermal plasma, electrochemical and photo-activated processes, and their combination, are viewed as sustainable approaches to increase reaction rates and shorten reaction times while enhancing yields and selectivities.

Based on the above considerations, submissions to this Special Issue are welcome in the form of original research papers, reviews, or communications that highlight promising recent research and novel trends in the field of heterogeneous catalytic oxidation or photocatalytic oxidation. Both selective and total oxidation reactions will be considered in this themed issue. They could either encompass the (photo)catalytic transformation of various organic compounds (alcohols, alkanes, alkenes, bio-derived sustainable feedstocks, lignocellulosic biomass, waste, etc.) to value-added chemicals or the (photo)catalytic removal/degradation of organic pollutants (dyes, aromatics, pesticides, pharmaceuticals, VOCs, CO, CH4, etc.). Reactions could be in liquid or gas phase, employing a variety of nanocatalysts (metal oxides, metals or organometallic complexes supported or not on inert oxides or (porous)carbons; zeolites; mesoporous materials) and various oxidants (O2, H2O2, O3, oxone, peroxydisulfate, etc.). The topic also concerns the development of new catalysts’ synthetic routes for the abovementioned (photo)catalytic reactions, as well as the establishment of structure–property relationships for the understanding of the reaction mechanisms. Moreover, studies dealing with the use of physical activation methods (e.g., ultrasound, microwave, ball-milling, non-thermal plasma, UV, electrochemistry) either for selective and total catalytic oxidation reactions or for the design of nanomaterials with improved characteristics and catalytic properties in view of the topic of this Special Issue are also very welcome. Both academic and industrial research studies are perfectly matched to this Special Issue dedicated to Heterogeneous Selective and Total Catalytic Oxidation.

Prof. Dr. Sabine Valange
Prof. Dr. Jacques Charles Védrine
Guest Editor

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Catalysts is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • heterogeneous catalysis
  • partial/selective oxidation
  • total oxidation
  • photocatalysis
  • liquid and gas phase
  • supported and unsupported catalysts (metal oxides, metals, organometallic complexes, nanocatalysts, zeolites, mesoporous materials, photocatalysts)
  • physical activation methods (e.g. ultrasound, microwave, ball-milling, non-thermal plasma, UV, electrochemistry)
  • water and air treatment
  • AOP (advanced oxidation process)

Published Papers (12 papers)

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Research

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14 pages, 1926 KiB  
Article
Hydrothermal Modification of TS-1 Zeolites with Organic Amines and Salts to Construct Highly Selective Catalysts for Cyclopentene Epoxidation
by Xin-Yu Chang, Yu-Ting Sun, Xiao-Jing Song, Xiao-Tong Yang, Yu-Qing Wu and Ming-Jun Jia
Catalysts 2022, 12(10), 1241; https://0-doi-org.brum.beds.ac.uk/10.3390/catal12101241 - 15 Oct 2022
Cited by 1 | Viewed by 1791
Abstract
Developing efficient heterogeneous catalysts for cyclic olefins epoxidation is highly attractive for meeting the growing need for various cyclic epoxides. Herein, hierarchical TS-1 zeolite with relatively abundant mesopores and less amount of surface hydroxyl groups was obtained by hydrothermal modification of an as-synthesized [...] Read more.
Developing efficient heterogeneous catalysts for cyclic olefins epoxidation is highly attractive for meeting the growing need for various cyclic epoxides. Herein, hierarchical TS-1 zeolite with relatively abundant mesopores and less amount of surface hydroxyl groups was obtained by hydrothermal modification of an as-synthesized TS-1 zeolite with a mixed solution of ammonia, tetrapropylammonium bromide (TPABr) and KCl. The post-modified TS-1 zeolite exhibited much higher catalytic activity (52% conversion) and epoxide selectivity (98%) for the epoxidation of cyclopentene than the conventional TS-1 zeolites. The excellent catalytic activity of the hierarchical TS-1 could be mainly assigned to the enhancement of the mass transport ability and the accessibility of the active Ti species, while the improvement of epoxidation selectivity may be mainly related to the introduction of a certain amount of K+ that can effectively modulate the coordination environment of Ti species as well as the polarity of the zeolite. This work demonstrated that a highly active and selective catalyst for the H2O2-mediated cyclopentene epoxidation could be obtained by concurrently generating mesopore and extinguishing the unfavorable defective hydroxyl groups through the simple hydrothermal treatment of the conventional TS-1 zeolite with a mixed base/salt solution. Full article
(This article belongs to the Special Issue Heterogeneous Selective and Total Catalytic Oxidation)
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15 pages, 1319 KiB  
Article
Synergistic Effect in Ag/Fe–MnO2 Catalysts for Ethanol Oxidation
by Ekaterina V. Kulchakovskaya, Svyatoslav S. Dotsenko, Leonarda F. Liotta, Valeria La Parola, Sergey I. Galanov, Olga I. Sidorova and Olga V. Vodyankina
Catalysts 2022, 12(8), 872; https://0-doi-org.brum.beds.ac.uk/10.3390/catal12080872 - 07 Aug 2022
Cited by 2 | Viewed by 1610
Abstract
Here we report the synergistic effect of OMS-2 catalysts tested in ethanol oxidation, and the effects produced by both the addition of an Fe modifier in the catalyst preparation stage, and the introduction of Ag on its surface by the impregnation method. To [...] Read more.
Here we report the synergistic effect of OMS-2 catalysts tested in ethanol oxidation, and the effects produced by both the addition of an Fe modifier in the catalyst preparation stage, and the introduction of Ag on its surface by the impregnation method. To analyze the action of each component, the Fe-modified, Ag-containing OMS-2 catalysts with different Mn/Fe ratios were prepared. Combined XPS and XRF elemental analysis confirms the states and distribution of the Ag- and Fe-containing species between the surface and bulk of the OMS-2 catalysts, which form highly dispersed Ag species on the surface of 0.05Fe–OMS-2, and are also incorporated into the OMS-2 crystalline lattice. The cooperative action of Ag and Fe modifiers improves both reoxidation ability (TPO results) and the amount of adsorbed oxygen species on the catalyst surface. The introduction of Ag to the OMS-2 and 0.05 Fe–OMS-2 surface allows a high level of activity (T80 = 150–155 °C) and selectivity (SAc80 = 93%) towards the acetaldehyde formation. Full article
(This article belongs to the Special Issue Heterogeneous Selective and Total Catalytic Oxidation)
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9 pages, 1373 KiB  
Communication
Activation of Peroxydisulfate by Bimetallic Nano Zero-Valent Iron for Waste-Activated Sludge Disintegration
by Barbara Socha, Daniele Silvestri, Klaudiusz Grübel, Vinod V. T. Padil, Mariusz Dudziak, Farshid Ghanbari, Miroslav Černík and Stanisław Wacławek
Catalysts 2022, 12(6), 590; https://0-doi-org.brum.beds.ac.uk/10.3390/catal12060590 - 28 May 2022
Viewed by 2114
Abstract
Waste-activated sludge (WAS) disintegration using peroxydisulfate (PDS) has attracted scientific attention over the past few years. Despite several advantages offered by a sulfate radical-advanced oxidation process, there are still too many downsides of this treatment that limit its facile large-scale application. This study [...] Read more.
Waste-activated sludge (WAS) disintegration using peroxydisulfate (PDS) has attracted scientific attention over the past few years. Despite several advantages offered by a sulfate radical-advanced oxidation process, there are still too many downsides of this treatment that limit its facile large-scale application. This study investigated whether modifying nano zero-valent iron (nZVI) with a second metal such as Ag and Cu enhanced the disruption of WAS. The disintegration efficiency was assessed using standard techniques, i.e., soluble chemical oxygen demand, Fourier-transform infrared spectroscopy and a scanning electron microscope. The bimetallics were shown to have an improved disintegration efficiency of > 2.5-fold compared with the untreated sample. Furthermore, nZVI/Ag was found to be more efficient than nZVI/Cu for PDS activation, which was validated by the higher ratio (3 and 2.5 for nZVI/Ag and nZVI/Cu, respectively) between the soluble extracellular polymeric substances and the bound extracellular polymeric substances (S-EPS/B-EPS). Similar conclusions were derived from a SEM analysis. The improved disintegration efficiency could be related to the enhanced electron transfer from nZVI to PDS or the intrinsic properties of silver, which was found to be one of the best activators for PDS under homogeneous conditions. We believe that this study deepens the understanding of PDS heterogeneous activation processes. Full article
(This article belongs to the Special Issue Heterogeneous Selective and Total Catalytic Oxidation)
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21 pages, 3620 KiB  
Article
Low Temperature Catalytic Oxidation of Ethanol Using Ozone over Manganese Oxide-Based Catalysts in Powdered and Monolithic Forms
by Houcine Touati, Sabine Valange, Marc Reinholdt, Catherine Batiot-Dupeyrat, Jean-Marc Clacens and Jean-Michel Tatibouët
Catalysts 2022, 12(2), 172; https://0-doi-org.brum.beds.ac.uk/10.3390/catal12020172 - 28 Jan 2022
Cited by 8 | Viewed by 2575
Abstract
Catalytic oxidation of low concentrations of ethanol was investigated in dry and humid air streams at low temperature (60 °C) over manganese oxide-based catalysts supported on a meso–macrostructured TiO2 using ozone as the oxidant. Ethanol was selected as a representative model VOC [...] Read more.
Catalytic oxidation of low concentrations of ethanol was investigated in dry and humid air streams at low temperature (60 °C) over manganese oxide-based catalysts supported on a meso–macrostructured TiO2 using ozone as the oxidant. Ethanol was selected as a representative model VOC present in indoor air, and its concentration was fixed to 10 ppm. For that purpose, a series of Mn/TiO2 powder and monolithic catalysts was prepared, some doped with 0.5 wt% Pd. Whatever the catalyst, the presence of water vapor in the gas phase had a beneficial effect on the conversion of ethanol and ozone. The Pd–Mn/TiO2 catalyst containing 0.5 wt% Pd and 5 wt% Mn exhibited superior oxidation efficiency to the Mn/TiO2 counterparts by increasing ozone decomposition (77%) while simultaneously increasing the selectivity to CO2 (85%). The selectivity to CO2 approached nearly 100% by increasing the amount of catalyst from 20 to 80 mg. In a further step, alumina wash-coated cordierite honeycomb monoliths were coated with the 0.5Pd–5Mn/TiO2 catalyst. Full conversion of ethanol to CO2 without residual O3 emitted (less than 10 ppb) could be attained, thereby demonstrating that the proposed Pd–Mn/TiO2 monolithic catalyst fulfills the specifications required for onboard systems. Full article
(This article belongs to the Special Issue Heterogeneous Selective and Total Catalytic Oxidation)
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15 pages, 2286 KiB  
Article
Ambient Temperature CO Oxidation Using Palladium–Platinum Bimetallic Catalysts Supported on Tin Oxide/Alumina
by James K. Aldridge, Louise R. Smith, David J. Morgan, Albert F. Carley, Mandy Humphreys, Michael J. Clarke, Patricia Wormald, Stuart H. Taylor and Graham J. Hutchings
Catalysts 2020, 10(11), 1223; https://0-doi-org.brum.beds.ac.uk/10.3390/catal10111223 - 22 Oct 2020
Cited by 5 | Viewed by 2373
Abstract
A series of Pt-based catalysts were synthesised and investigated for ambient temperature CO oxidation with the aim to increase catalytic activity and improve moisture resistance through support modification. Initially, bimetallic PtPd catalysts supported on alumina were found to exhibit superior catalytic activity compared [...] Read more.
A series of Pt-based catalysts were synthesised and investigated for ambient temperature CO oxidation with the aim to increase catalytic activity and improve moisture resistance through support modification. Initially, bimetallic PtPd catalysts supported on alumina were found to exhibit superior catalytic activity compared with their monometallic counterparts for the reaction. Following an investigation into the effect of Pt/Pd ratio, a composition of 0.1% Pt/0.4% Pd was selected for further studies. Following this, SnO2/Al2O3 supports were synthesised from a variety of tin oxide sources. Catalytic activity was improved using sodium stannate and tin oxalate precursors compared with a traditional tin oxide slurry. Catalytic activity versus tin concentration was found to vary significantly across the three precursors, which was subsequently investigated by X-ray photoelectron spectroscopy (XPS) and energy-dispersive X-ray spectroscopy (EDX). Full article
(This article belongs to the Special Issue Heterogeneous Selective and Total Catalytic Oxidation)
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24 pages, 4439 KiB  
Article
Highly Active Transition Metal-Promoted CuCeMgAlO Mixed Oxide Catalysts Obtained from Multicationic LDH Precursors for the Total Oxidation of Methane
by Hussein Mahdi S. Al-Aani, Mihaela M. Trandafir, Ioana Fechete, Lucia N. Leonat, Mihaela Badea, Cătălin Negrilă, Ionel Popescu, Mihaela Florea and Ioan-Cezar Marcu
Catalysts 2020, 10(6), 613; https://0-doi-org.brum.beds.ac.uk/10.3390/catal10060613 - 01 Jun 2020
Cited by 6 | Viewed by 2941
Abstract
To improve the catalytic performance of an active layered double hydroxide (LDH)-derived CuCeMgAlO mixed oxide catalyst in the total oxidation of methane, it was promoted with different transition-metal cations. Thus, two series of multicationic mixed oxides were prepared by the thermal decomposition at [...] Read more.
To improve the catalytic performance of an active layered double hydroxide (LDH)-derived CuCeMgAlO mixed oxide catalyst in the total oxidation of methane, it was promoted with different transition-metal cations. Thus, two series of multicationic mixed oxides were prepared by the thermal decomposition at 750 °C of their corresponding LDH precursors synthesized by coprecipitation at constant pH of 10 under ambient atmosphere. The first series of catalysts consisted of four M(3)CuCeMgAlO mixed oxides containing 3 at.% M (M = Mn, Fe, Co, Ni), 15 at.% Cu, 10 at.% Ce (at.% with respect to cations), and with Mg/Al atomic ratio fixed to 3. The second series consisted of four Co(x)CuCeMgAlO mixed oxides with x = 1, 3, 6, and 9 at.% Co, while keeping constant the Cu and Ce contents and the Mg/Al atomic ratio. All the mixed oxides were characterized by powder X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM) coupled with X-ray energy dispersion analysis (EDX), X-ray photoelectron spectroscopy (XPS), nitrogen adsorption-desorption at −196 °C, temperature-programmed reduction under hydrogen (H2-TPR), and diffuse reflectance UV-VIS spectroscopy (DR UV-VIS), while thermogravimetric and differential thermal analyses (TG-DTG-DTA) together with XRD were used for the LDH precursors. The catalysts were evaluated in the total oxidation of methane, a test reaction for volatile organic compounds (VOC) abatement. Their catalytic performance was explained in correlation with their physicochemical properties and was compared with that of a reference Pd/Al2O3 catalyst. Among the mixed oxides studied, Co(3)CuCeMgAlO was found to be the most active catalyst, with a temperature corresponding to 50% methane conversion (T50) of 438 °C, which was only 19 °C higher than that of a reference Pd/Al2O3 catalyst. On the other hand, this T50 value was ca. 25 °C lower than that observed for the unpromoted CuCeMgAlO system, accounting for the improved performance of the Co-promoted catalyst, which also showed a good stability on stream. Full article
(This article belongs to the Special Issue Heterogeneous Selective and Total Catalytic Oxidation)
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17 pages, 3406 KiB  
Article
Synergistic Effect in Au-Cu Bimetallic Catalysts for the Valorization of Lignin-Derived Compounds
by Marta Stucchi, Sofia Capelli, Simone Cardaci, Stefano Cattaneo, Andrea Jouve, Andrea Beck, György Sáfrán, Claudio Evangelisti, Alberto Villa and Laura Prati
Catalysts 2020, 10(3), 332; https://0-doi-org.brum.beds.ac.uk/10.3390/catal10030332 - 16 Mar 2020
Cited by 12 | Viewed by 3288
Abstract
The selective oxidation of veratryl alcohol as lignin-derived compound was studied under mild conditions, using Au-Cu catalysts synthesized from pre-formed nanoparticles with different Au:Cu molar ratios. Bimetallic catalysts show higher activity compared to monometallic counterparts, highlighting a clear synergistic effect. By comparing the [...] Read more.
The selective oxidation of veratryl alcohol as lignin-derived compound was studied under mild conditions, using Au-Cu catalysts synthesized from pre-formed nanoparticles with different Au:Cu molar ratios. Bimetallic catalysts show higher activity compared to monometallic counterparts, highlighting a clear synergistic effect. By comparing the physico-chemical surface properties of catalysts supported on carbon and Al2O3, we were able to establish a strong support effect, with alumina-based catalysts being more active than carbon-supported ones. Moreover, TEM and X-ray photoelectron spectroscopy (XPS) analyses showed a different composition of nanoparticles (NPs) and metal exposure, and we established that Au is the active phase of the reaction. The co-presence of Au and Cu species, and their different interaction with the support, enabled obtaining more than 70% conversion of veratryl alcohol to veratryl aldehyde as a unique product. Moreover, the Au1Cu1 supported on alumina catalyst was recovered by filtration and reused without significant loss of activity and selectivity up to four times. Full article
(This article belongs to the Special Issue Heterogeneous Selective and Total Catalytic Oxidation)
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12 pages, 3756 KiB  
Article
Effect of Molybdenum on the Activity Temperature Enlarging of Mn-Based Catalyst for Mercury Oxidation
by Bo Zhao, Xiaojiong Zhao, Yangshuo Liang, Yu Wang, Linbo Qin and Wangsheng Chen
Catalysts 2020, 10(2), 147; https://0-doi-org.brum.beds.ac.uk/10.3390/catal10020147 - 22 Jan 2020
Cited by 5 | Viewed by 2157
Abstract
The MnO2/TiO2 (TM5) catalyst modified by molybdenum was used for mercury oxidation at different temperatures in a fixed-bed reactor. The addition of molybdenum into TM5 was identified as significantly enlarging the optimal temperature range for mercury oxidation. [...] Read more.
The MnO2/TiO2 (TM5) catalyst modified by molybdenum was used for mercury oxidation at different temperatures in a fixed-bed reactor. The addition of molybdenum into TM5 was identified as significantly enlarging the optimal temperature range for mercury oxidation. The optimal mercury oxidation temperature of TM5 was only 200 °C, with an oxidation efficiency of 95%. However, the mercury oxidation efficiency of TM5 was lower than 60% at other temperatures. As for MnO2–MoO3/TiO2 (TM5Mo5), the mercury oxidation efficiency was above 80% at 200–350 °C. In particular at 250 °C, the mercury oxidation efficiency of TM5Mo5 was over 93%. Otherwise, the gaseous O2, which could supplement the lattice oxygen in the catalytic reaction, played an important role in the process of mercury oxidation over TM5Mo5. The results of X-ray photoelectron spectroscopy (XPS) suggested that mercury oxidized by O2 over TM5Mo5 followed the Mars–Maessen mechanism. Full article
(This article belongs to the Special Issue Heterogeneous Selective and Total Catalytic Oxidation)
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Review

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21 pages, 2431 KiB  
Review
Recent Advances in the Catalytic Treatment of Volatile Organic Compounds: A Review Based on the Mixture Effect
by Guillaume Rochard, Lilian Olivet, Mariebelle Tannous, Christophe Poupin, Stéphane Siffert and Renaud Cousin
Catalysts 2021, 11(10), 1218; https://0-doi-org.brum.beds.ac.uk/10.3390/catal11101218 - 09 Oct 2021
Cited by 20 | Viewed by 3239
Abstract
Catalytic total oxidation is an efficient technique for treating VOCs, which are mainly emitted by solvent-based industrial processes. However, studies of the catalytic oxidation of VOCs in combination with other pollutants are very limited, despite the fact that this is a key step [...] Read more.
Catalytic total oxidation is an efficient technique for treating VOCs, which are mainly emitted by solvent-based industrial processes. However, studies of the catalytic oxidation of VOCs in combination with other pollutants are very limited, despite the fact that this is a key step of knowledge before industrial application. During the oxidation reaction, the behavior of a molecule may change depending on the reaction mixture. For the treatment of an effluent loaded with VOCs, it is necessary to carefully select not only the catalytic material to be used but also the reaction conditions. Indeed, the catalytic oxidation of a component in a VOCs mixture is not predicted solely from the behavior of individual component. Thus, the objective of this small review is to carry out a study on the effect observed in the case of the oxidation of a VOCs mixture or in the presence of water, NOX or sulfur compounds. Full article
(This article belongs to the Special Issue Heterogeneous Selective and Total Catalytic Oxidation)
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30 pages, 11284 KiB  
Review
Review on Alternative Route to Acrolein through Oxidative Coupling of Alcohols
by Vincent Folliard, Jacopo de Tommaso and Jean-Luc Dubois
Catalysts 2021, 11(2), 229; https://0-doi-org.brum.beds.ac.uk/10.3390/catal11020229 - 09 Feb 2021
Cited by 3 | Viewed by 3649
Abstract
Oxidative coupling of alcohols using methanol and ethanol, which can both be made renewable, is an attractive route to produce acrolein (propenaldehyde) in a single-step process. Currently acrolein is produced by direct oxidation of fossil propylene, and catalytic double dehydration of glycerol has [...] Read more.
Oxidative coupling of alcohols using methanol and ethanol, which can both be made renewable, is an attractive route to produce acrolein (propenaldehyde) in a single-step process. Currently acrolein is produced by direct oxidation of fossil propylene, and catalytic double dehydration of glycerol has been also investigated up to pilot scale. Although glycerol is an attractive feedstock, it suffers of several drawbacks. Addressing the limitations of both routes, the oxidative coupling of alcohols combines an exothermic oxidation and cross-aldolization. The best performing catalysts so far combine redox and acid/base sites. Reviewing the academic and patent literature, the present paper also addresses the economic analysis, to highlight the potential of this reaction at a yield from 70%, and at two different plant scales. The analysis has been made to guide further research, with the remaining technical problems to solve. Improved selectivity contributing to reduce the amount of equipment and the investment cost should be the prime target. Full article
(This article belongs to the Special Issue Heterogeneous Selective and Total Catalytic Oxidation)
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Other

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24 pages, 7768 KiB  
Perspective
Immobilization of Polyoxometalates on Carbon Nanotubes: Tuning Catalyst Activity, Selectivity and Stability in H2O2-Based Oxidations
by Vasilii Yu. Evtushok, Vladimir A. Lopatkin, Olga Yu. Podyacheva and Oxana A. Kholdeeva
Catalysts 2022, 12(5), 472; https://0-doi-org.brum.beds.ac.uk/10.3390/catal12050472 - 22 Apr 2022
Cited by 4 | Viewed by 2449
Abstract
In recent years, carbon nanotubes (CNTs), including N-doped ones (N-CNTs), have received significant attention as supports for the construction of heterogeneous catalysts. In this work, we summarize our progress in the application of (N)-CNTs for immobilization of anionic metal-oxygen clusters or polyoxometalates (POMs) [...] Read more.
In recent years, carbon nanotubes (CNTs), including N-doped ones (N-CNTs), have received significant attention as supports for the construction of heterogeneous catalysts. In this work, we summarize our progress in the application of (N)-CNTs for immobilization of anionic metal-oxygen clusters or polyoxometalates (POMs) and use of (N)-CNTs-supported POM as catalysts for liquid-phase selective oxidation of organic compounds with the green oxidant–aqueous hydrogen peroxide. We discuss here the main factors, which favor adsorption of POMs on (N)-CNTs and ensure a quasi-molecular dispersion of POM on the surface and their strong attachment to the support. The effects of the POM nature, N-doping of CNTs, acid additives, and other factors on the POM immobilization process and catalytic activity/selectivity of the (N)-CNTs-immobilized POMs are analyzed. Particular attention is drawn to the critical issue of the catalyst stability and reusability. The scope and limitations of the POM/(N)-CNTs catalysts in H2O2-based selective oxidations are discussed. Full article
(This article belongs to the Special Issue Heterogeneous Selective and Total Catalytic Oxidation)
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23 pages, 5140 KiB  
Perspective
Metal-Organic Frameworks in Oxidation Catalysis with Hydrogen Peroxide
by Oxana Kholdeeva and Nataliya Maksimchuk
Catalysts 2021, 11(2), 283; https://0-doi-org.brum.beds.ac.uk/10.3390/catal11020283 - 21 Feb 2021
Cited by 34 | Viewed by 5273
Abstract
In recent years, metal–organic frameworks (MOFs) have received increasing attention as selective oxidation catalysts and supports for their construction. In this short review paper, we survey recent findings concerning use of MOFs in heterogeneous liquid-phase selective oxidation catalysis with the green oxidant–aqueous hydrogen [...] Read more.
In recent years, metal–organic frameworks (MOFs) have received increasing attention as selective oxidation catalysts and supports for their construction. In this short review paper, we survey recent findings concerning use of MOFs in heterogeneous liquid-phase selective oxidation catalysis with the green oxidant–aqueous hydrogen peroxide. MOFs having outstanding thermal and chemical stability, such as Cr(III)-based MIL-101, Ti(IV)-based MIL-125, Zr(IV)-based UiO-66(67), Zn(II)-based ZIF-8, and some others, will be in the main focus of this work. The effects of the metal nature and MOF structure on catalytic activity and oxidation selectivity are analyzed and the mechanisms of hydrogen peroxide activation are discussed. In some cases, we also make an attempt to analyze relationships between liquid-phase adsorption properties of MOFs and peculiarities of their catalytic performance. Attempts of using MOFs as supports for construction of single-site catalysts through their modification with heterometals will be also addressed in relation to the use of such catalysts for activation of H2O2. Special attention is given to the critical issues of catalyst stability and reusability. The scope and limitations of MOF catalysts in H2O2-based selective oxidation are discussed. Full article
(This article belongs to the Special Issue Heterogeneous Selective and Total Catalytic Oxidation)
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