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Advanced Materials in Catalysis and Adsorption

A special issue of Materials (ISSN 1996-1944). This special issue belongs to the section "Catalytic Materials".

Deadline for manuscript submissions: closed (20 September 2022) | Viewed by 32285

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Special Issue Editor

Department of Materials Science and Functional Materials, Boreskov Institute of Catalysis, 630090 Novosibirsk, Russia
Interests: heterogeneous catalysis; nanotechnology; carbon nanofibers; functionalized carbon materials; self-organized catalysts; hierarchical composites; nanocrystalline oxides; oxidative dehydrogenation; three-way catalysts; alloys; catalytic decomposition; chemical vapor deposition; environmental catalysis; metal dusting and corrosion
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Special Issue Information

Dear Colleagues,

Achievements in modern materials science have produced new classes of advanced materials. Due to their unique properties, such materials attract great attention in various fields of application. The present Special Issue is focused on two of these application areas, heterogeneous catalysis and adsorption. In fact, structure–activity relationships in functional materials and nanomaterials and catalytically and adsorption-mediated transformations of materials are subjects of intense research. Attention is payed in particular to physicochemical experiments, molecular design, simulations of materials and their interactions with adsorptive and reaction media.

Topics of interest of the Special Issue “Advanced Materials in Catalysis and Adsorption” include functional materials such as modified nanostructured oxides, porous and sponge-like alloys, electrides and electron-conductive materials, catalytically derived materials, carbon nanostructured materials, carbon–metal hybrids, materials with a hierarchical porous structure, 2D and 3D self-assembled systems, zeolites (zeotypes), ordered mesoporous materials, alumoposphates, metal-organic and covalent organic frameworks, and other ordered materials of prospective use in catalysis and adsorption.

We kindly invite you to submit a manuscript(s) for this Special Issue. Full papers, communications, and reviews are all welcome.

Dr. Ilya V. Mishakov
Guest Editor

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Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2600 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

  • nanostructured oxides
  • porous and sponge-like alloys
  • electrides and electron-conductive materials
  • catalytically derived materials
  • hybrid carbon-metal catalysts
  • materials with hierarchical porous structure
  • 2D and 3D self-assembled systems
  • zeotypes and other ordered materials
  • metal-organic frameworks in catalysis
  • adsorption induced porosity

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Published Papers (19 papers)

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Editorial

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4 pages, 200 KiB  
Editorial
Editorial for Special Issue “Advanced Materials in Catalysis and Adsorption”
by Ilya V. Mishakov
Materials 2023, 16(7), 2895; https://0-doi-org.brum.beds.ac.uk/10.3390/ma16072895 - 05 Apr 2023
Viewed by 874
Abstract
This Special Issue aims to cover the latest research on the design and development of advanced materials for adsorption and catalytic applications [...] Full article
(This article belongs to the Special Issue Advanced Materials in Catalysis and Adsorption)

Research

Jump to: Editorial, Review

11 pages, 3887 KiB  
Article
Synthesis of Boron-Doped Carbon Nanomaterial
by Vladimir V. Chesnokov, Igor P. Prosvirin, Evgeny Yu. Gerasimov and Aleksandra S. Chichkan
Materials 2023, 16(5), 1986; https://0-doi-org.brum.beds.ac.uk/10.3390/ma16051986 - 28 Feb 2023
Cited by 3 | Viewed by 1658
Abstract
A new method for the synthesis of boron-doped carbon nanomaterial (B-carbon nanomaterial) has been developed. First, graphene was synthesized using the template method. Magnesium oxide was used as the template that was dissolved with hydrochloric acid after the graphene deposition on its surface. [...] Read more.
A new method for the synthesis of boron-doped carbon nanomaterial (B-carbon nanomaterial) has been developed. First, graphene was synthesized using the template method. Magnesium oxide was used as the template that was dissolved with hydrochloric acid after the graphene deposition on its surface. The specific surface area of the synthesized graphene was equal to 1300 m2/g. The suggested method includes the graphene synthesis via the template method, followed by the deposition of an additional graphene layer doped with boron in an autoclave at 650 °C, using a mixture of phenylboronic acid, acetone, and ethanol. After this carbonization procedure, the mass of the graphene sample increased by 70%. The properties of B-carbon nanomaterial were studied using X-ray photoelectron spectroscopy (XPS), high-resolution transmission electron microscopy (HRTEM), Raman spectroscopy, and adsorption-desorption techniques. The deposition of an additional graphene layer doped with boron led to an increase of the graphene layer thickness from 2–4 to 3–8 monolayers, and a decrease of the specific surface area from 1300 to 800 m2/g. The boron concentration in B-carbon nanomaterial determined by different physical methods was about 4 wt.%. Full article
(This article belongs to the Special Issue Advanced Materials in Catalysis and Adsorption)
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22 pages, 13623 KiB  
Article
Efficient Production of Segmented Carbon Nanofibers via Catalytic Decomposition of Trichloroethylene over Ni-W Catalyst
by Arina R. Potylitsyna, Yuliya V. Rudneva, Yury I. Bauman, Pavel E. Plyusnin, Vladimir O. Stoyanovskii, Evgeny Y. Gerasimov, Aleksey A. Vedyagin, Yury V. Shubin and Ilya V. Mishakov
Materials 2023, 16(2), 845; https://0-doi-org.brum.beds.ac.uk/10.3390/ma16020845 - 15 Jan 2023
Cited by 4 | Viewed by 1235
Abstract
The catalytic utilization of chlorine-organic wastes remains of extreme importance from an ecological point of view. Depending on the molecular structure of the chlorine-substituted hydrocarbon (presence of unsaturated bonds, intermolecular chlorine-to-hydrogen ratio), the features of its catalytic decomposition can be significantly different. Often, [...] Read more.
The catalytic utilization of chlorine-organic wastes remains of extreme importance from an ecological point of view. Depending on the molecular structure of the chlorine-substituted hydrocarbon (presence of unsaturated bonds, intermolecular chlorine-to-hydrogen ratio), the features of its catalytic decomposition can be significantly different. Often, 1,2-dichloroethane is used as a model substrate. In the present work, the catalytic decomposition of trichloroethylene (C2HCl3) over microdispersed 100Ni and 96Ni-4W with the formation of carbon nanofibers (CNF) was studied. Catalysts were obtained by a co-precipitation of complex salts followed by reductive thermolysis. The disintegration of the initial bulk alloy driven by its interaction with the reaction mixture C2HCl3/H2/Ar entails the formation of submicron active particles. It has been established that the optimal activity of the pristine Ni catalyst and the 96Ni-4W alloy is provided in temperature ranges of 500–650 °C and 475–725 °C, respectively. The maximum yield of CNF for 2 h of reaction was 63 g/gcat for 100Ni and 112 g/gcat for 96Ni-4W catalyst. Longevity tests showed that nickel undergoes fast deactivation (after 3 h), whereas the 96Ni-4W catalyst remains active for 7 h of interaction. The effects of the catalyst’s composition and the reaction temperature upon the structural and morphological characteristics of synthesized carbon nanofibers were investigated by X-ray diffraction analysis, Raman spectroscopy, and electron microscopies. The initial stages of the carbon erosion process were precisely examined by transmission electron microscopy coupled with elemental mapping. The segmented structure of CNF was found to be prevailing in a range of 500–650 °C. The textural parameters of carbon product (SBET and Vpore) were shown to reach maximum values (374 m2/g and 0.71 cm3/g, respectively) at the reaction temperature of 550 °C. Full article
(This article belongs to the Special Issue Advanced Materials in Catalysis and Adsorption)
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15 pages, 4289 KiB  
Article
Comparative Study on Carbon Erosion of Nickel Alloys in the Presence of Organic Compounds under Various Reaction Conditions
by Alexander M. Volodin, Roman M. Kenzhin, Yury I. Bauman, Sofya D. Afonnikova, Arina R. Potylitsyna, Yury V. Shubin, Ilya V. Mishakov and Aleksey A. Vedyagin
Materials 2022, 15(24), 9033; https://0-doi-org.brum.beds.ac.uk/10.3390/ma15249033 - 17 Dec 2022
Cited by 1 | Viewed by 1015
Abstract
The processes of carbon erosion of nickel alloys during the catalytic pyrolysis of organic compounds with the formation of carbon nanofibers in a flow-through reactor as well as under reaction conditions in a close volume (Reactions under Autogenic Pressure at Elevated Temperature, RAPET) [...] Read more.
The processes of carbon erosion of nickel alloys during the catalytic pyrolysis of organic compounds with the formation of carbon nanofibers in a flow-through reactor as well as under reaction conditions in a close volume (Reactions under Autogenic Pressure at Elevated Temperature, RAPET) were studied. The efficiency of the ferromagnetic resonance method to monitor the appearance of catalytically active nickel particles in these processes has been shown. As found, the interaction of bulk Ni-Cr alloy with the reaction medium containing halogenated hydrocarbons (1,2-dichloroethane, 1-iodobutane, 1-bromobutane) results in the appearance of ferromagnetic particles of similar dimensions (~200–300 nm). In the cases of hexachlorobenzene and hexafluorobenzene, the presence of a hydrogen source (hexamethylbenzene) in the reaction mixture was shown to be highly required. The microdispersed samples of Ni-Cu and Ni-Mo alloys were prepared by mechanochemical alloying of powders and by reductive thermolysis of salts-precursors, accordingly. Their interaction with polymers (polyethylene and polyvinyl chloride) under RAPET conditions and with ethylene and 1,2-dichloroethane in a flow-through reactor are comparatively studied as well. According to microscopic data, the morphology of the formed carbon nanofibers is affected by the alloy composition and by the nature of the used organic substrate. Full article
(This article belongs to the Special Issue Advanced Materials in Catalysis and Adsorption)
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19 pages, 6333 KiB  
Article
Synthesis of Chlorine- and Nitrogen-Containing Carbon Nanofibers for Water Purification from Chloroaromatic Compounds
by Anna M. Ozerova, Arina R. Potylitsyna, Yury I. Bauman, Elena S. Tayban, Inna L. Lipatnikova, Anna V. Nartova, Aleksey A. Vedyagin, Ilya V. Mishakov, Yury V. Shubin and Olga V. Netskina
Materials 2022, 15(23), 8414; https://0-doi-org.brum.beds.ac.uk/10.3390/ma15238414 - 25 Nov 2022
Cited by 4 | Viewed by 2044
Abstract
Chlorine- and nitrogen-containing carbon nanofibers (CNFs) were obtained by combined catalytic pyrolysis of trichloroethylene (C2HCl3) and acetonitrile (CH3CN). Their efficiency in the adsorption of 1,2-dichlorobenzene (1,2-DCB) from water has been studied. The synthesis of CNFs [...] Read more.
Chlorine- and nitrogen-containing carbon nanofibers (CNFs) were obtained by combined catalytic pyrolysis of trichloroethylene (C2HCl3) and acetonitrile (CH3CN). Their efficiency in the adsorption of 1,2-dichlorobenzene (1,2-DCB) from water has been studied. The synthesis of CNFs was carried out over self-dispersing nickel catalyst at 600 °C. The produced CNFs possess a well-defined segmented structure, high specific surface area (~300 m2/g) and high porosity (0.5–0.7 cm3/g). The addition of CH3CN into the reaction mixture allows the introduction of nitrogen into the CNF structure and increases the volume of mesopores. As a result, the capacity of CNF towards adsorption of 1,2-DCB from its aqueous solution increased from 0.41 to 0.57 cm3/g. Regardless of the presence of N, the CNF samples exhibited a degree of 1,2-DCB adsorption from water–organic emulsion exceeding 90%. The adsorption process was shown to be well described by the Dubinin–Astakhov equation. The regeneration of the used CNF adsorbent through liquid-phase hydrodechlorination was also investigated. For this purpose, Pd nanoparticles (1.5 wt%) were deposited on the CNF surface to form the adsorbent with catalytic function. The presence of palladium was found to have a slight effect on the adsorption capacity of CNF. Further regeneration of the adsorbent-catalyst via hydrodechlorination of adsorbed 1,2-DCB was completed within 1 h with 100% conversion. The repeated use of regenerated adsorbent-catalysts for purification of solutions after the first cycle of adsorption ensures almost complete removal of 1,2-DCB. Full article
(This article belongs to the Special Issue Advanced Materials in Catalysis and Adsorption)
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19 pages, 123621 KiB  
Article
Effect of Pretreatment with Acids on the N-Functionalization of Carbon Nanofibers Using Melamine
by Tatyana A. Maksimova, Ilya V. Mishakov, Yury I. Bauman, Artem B. Ayupov, Maksim S. Mel’gunov, Aleksey M. Dmitrachkov, Anna V. Nartova, Vladimir O. Stoyanovskii and Aleksey A. Vedyagin
Materials 2022, 15(22), 8239; https://0-doi-org.brum.beds.ac.uk/10.3390/ma15228239 - 20 Nov 2022
Cited by 5 | Viewed by 1366
Abstract
Nowadays, N-functionalized carbon nanomaterials attract a growing interest. The use of melamine as a functionalizing agent looks prospective from environmental and cost points of view. Moreover, the melamine molecule contains a high amount of nitrogen with an atomic ratio C/N of 1/2. In [...] Read more.
Nowadays, N-functionalized carbon nanomaterials attract a growing interest. The use of melamine as a functionalizing agent looks prospective from environmental and cost points of view. Moreover, the melamine molecule contains a high amount of nitrogen with an atomic ratio C/N of 1/2. In present work, the initial carbon nanofibers (CNFs) were synthesized via catalytic pyrolysis of ethylene over microdispersed Ni–Cu alloy. The CNF materials were pretreated with 12% hydrochloric acid or with a mixture of concentrated nitric and sulfuric acids, which allowed etching of the metals from the fibers and oxidizing of the fibers’ surface. Finally, the CNFs were N-functionalized via their impregnation with a melamine solution and thermolysis in an inert atmosphere. According to the microscopic data, the initial structure of the CNFs remained the same after the pretreatment and post-functionalization procedures. At the same time, the surface of the N-functionalized CNFs became more defective. The textural properties of the materials were also affected. In the case of the oxidative treatment with a mixture of acids, the highest content of the surface oxygen of 11.8% was registered by X-ray photoelectron spectroscopy. The amount of nitrogen introduced during the post-functionalization of CNFs with melamine increased from 1.4 to 4.3%. Along with this, the surface oxygen concentration diminished to 6.4%. Full article
(This article belongs to the Special Issue Advanced Materials in Catalysis and Adsorption)
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20 pages, 5485 KiB  
Article
A New Insight into the Mechanisms Underlying the Discoloration, Sorption, and Photodegradation of Methylene Blue Solutions with and without BNOx Nanocatalysts
by Andrei T. Matveev, Liubov A. Varlamova, Anton S. Konopatsky, Denis V. Leybo, Ilia N. Volkov, Pavel B. Sorokin, Xiaosheng Fang and Dmitry V. Shtansky
Materials 2022, 15(22), 8169; https://0-doi-org.brum.beds.ac.uk/10.3390/ma15228169 - 17 Nov 2022
Cited by 3 | Viewed by 1666
Abstract
Methylene blue (MB) is widely used as a test material in photodynamic therapy and photocatalysis. These applications require an accurate determination of the MB concentration as well as the factors affecting the temporal evolution of the MB concentration. Optical absorbance is the most [...] Read more.
Methylene blue (MB) is widely used as a test material in photodynamic therapy and photocatalysis. These applications require an accurate determination of the MB concentration as well as the factors affecting the temporal evolution of the MB concentration. Optical absorbance is the most common method used to estimate MB concentration. This paper presents a detailed study of the dependence of the optical absorbance of aqueous methylene blue (MB) solutions in a concentration range of 0.5 to 10 mg·L−1. The nonlinear behavior of optical absorbance as a function of MB concentration is described for the first time. A sharp change in optical absorption is observed in the range of MB concentrations from 3.33 to 4.00 mg·L−1. Based on the analysis of the absorption spectra, it is concluded that this is due to the formation of MB dimers and trimers in the specific concentration range. For the first time, a strong, thermally induced discoloration effect of the MB solution under the influence of visible and sunlight was revealed: the simultaneous illumination and heating of MB solutions from 20 to 80 °C leads to a twofold decrease in the MB concentration in the solution. Exposure to sunlight for 120 min at a temperature of 80 °C led to the discoloration of the MB solution by more than 80%. The thermally induced discoloration of MB solutions should be considered in photocatalytic experiments when tested solutions are not thermally stabilized and heated due to irradiation. We discuss whether MB is a suitable test material for photocatalytic experiments and consider this using the example of a new photocatalytic material—boron oxynitride (BNOx) nanoparticles—with 4.2 and 6.5 at.% of oxygen. It is shown that discoloration is a complex process and includes the following mechanisms: thermally induced MB photodegradation, MB absorption on BNOx NPs, self-sensitizing MB photooxidation, and photocatalytic MB degradation. Careful consideration of all these processes makes it possible to determine the photocatalytic contribution to the discoloration process when using MB as a test material. The photocatalytic activity of BNOx NPs containing 4.2 and 6.5 at.% of oxygen, estimated at ~440 μmol·g−1·h−1. The obtained results are discussed based on the results of DFT calculations considering the effect of MB sorption on its self-sensitizing photooxidation activity. A DFT analysis of the MB sorption capacity with BNOx NPs shows that surface oxygen defects prevent the sorption of MB molecules due to their planar orientation over the BNOx surface. To enhance the sorption capacity, surface oxygen defects should be eliminated. Full article
(This article belongs to the Special Issue Advanced Materials in Catalysis and Adsorption)
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12 pages, 2670 KiB  
Article
Nonstoichiometry Defects in Double Oxides of the A2BO4-Type
by Aleksandr S. Gorkusha, Sergey V. Tsybulya, Svetlana V. Cherepanova, Evgeny Y. Gerasimov and Svetlana N. Pavlova
Materials 2022, 15(21), 7642; https://0-doi-org.brum.beds.ac.uk/10.3390/ma15217642 - 31 Oct 2022
Cited by 3 | Viewed by 1240
Abstract
Double oxides with the structure of the Ruddlesden–Popper (R-P) layered perovskite An+1BnO3n+1 attract attention as materials for various electrochemical devices, selective oxygen-permeable ceramic membranes, and catalytic oxidative reactions. In particular, Sr2TiO4 layered perovskite is considered [...] Read more.
Double oxides with the structure of the Ruddlesden–Popper (R-P) layered perovskite An+1BnO3n+1 attract attention as materials for various electrochemical devices, selective oxygen-permeable ceramic membranes, and catalytic oxidative reactions. In particular, Sr2TiO4 layered perovskite is considered a promising catalyst in the oxidative coupling of methane. Our high-resolution transmission electron microscopy (HRTEM) studies of Sr2TiO4 samples synthesized using various methods have shown that their structure often contains planar defects disturbing the periodicity of layer alternation. This is due to the crystal-chemical features of the R-P layered perovskite-like oxides whose structure is formed by n consecutive layers of perovskite (ABO3)n in alternating with layers of rock-salt type (AO) in various ways along the c crystallographic direction. Planar defects can arise due to a periodicity violation of the layers alternation that also leads to a violation of the synthesized phase stoichiometry. In the present work, a crystallochemical analysis of the possible structure of planar defects is carried out, structures containing defects are modeled, and the effect of such defects on the X-ray diffraction patterns of oxides of the A2BO4 type using Sr2TiO4 is established as an example. For the calculations, we used the method of constructing probabilistic models of one-dimensionally disordered structures. For the first time, the features of diffraction were established, and an approach was demonstrated for determining the concentration of layer alternation defects applicable to layered perovskite-like oxides of the A2BO4 type of any chemical composition. A relation has been established between the concentration of planar defects and the real chemical composition (nonstoichiometry) of the Sr2TiO4 phase. The presence of defects leads to the Ti enrichment of particle volume and, consequently, to the enrichment of the surface with Sr. The latter, in turn, according to the data of a number of authors, can serve as an explanation for the catalytic activity of Sr2TiO4 in the oxidative coupling of methane. Full article
(This article belongs to the Special Issue Advanced Materials in Catalysis and Adsorption)
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12 pages, 1973 KiB  
Article
Robust Porous TiN Layer for Improved Oxygen Evolution Reaction Performance
by Gaoyang Liu, Faguo Hou, Xindong Wang and Baizeng Fang
Materials 2022, 15(21), 7602; https://0-doi-org.brum.beds.ac.uk/10.3390/ma15217602 - 29 Oct 2022
Cited by 7 | Viewed by 1410
Abstract
The poor reversibility and slow reaction kinetics of catalytic materials seriously hinder the industrialization process of proton exchange membrane (PEM) water electrolysis. It is necessary to develop high-performance and low-cost electrocatalysts to reduce the loss of reaction kinetics. In this study, a novel [...] Read more.
The poor reversibility and slow reaction kinetics of catalytic materials seriously hinder the industrialization process of proton exchange membrane (PEM) water electrolysis. It is necessary to develop high-performance and low-cost electrocatalysts to reduce the loss of reaction kinetics. In this study, a novel catalyst support featured with porous surface structure and good electronic conductivity was successfully prepared by surface modification via a thermal nitriding method under ammonia atmosphere. The morphology and composition characterization-confirmed that a TiN layer with granular porous structure and internal pore-like defects was established on the Ti sheet. Meanwhile, the conductivity measurements showed that the in-plane electronic conductivity of the as-developed material increased significantly to 120.8 S cm−1. After IrOx was loaded on the prepared TiN-Ti support, better dispersion of the active phase IrOx, lower ohmic resistance, and faster charge transfer resistance were verified, and accordingly, more accessible catalytic active sites on the catalytic interface were developed as revealed by the electrochemical characterizations. Compared with the IrOx/Ti, the as-obtained IrOx/TiN-Ti catalyst demonstrated remarkable electrocatalytic activity (η10 mA cm2 = 302 mV) and superior stability (overpotential degradation rate: 0.067 mV h−1) probably due to the enhanced mass adsorption and transport, good dispersion of the supported active phase IrOx, increased electronic conductivity and improved corrosion resistance provided by the TiN-Ti support. Full article
(This article belongs to the Special Issue Advanced Materials in Catalysis and Adsorption)
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18 pages, 3581 KiB  
Article
The Study of Thermal Stability of Mn-Zr-Ce, Mn-Ce and Mn-Zr Oxide Catalysts for CO Oxidation
by T. N. Afonasenko, D. V. Glyzdova, V. L. Yurpalov, V. P. Konovalova, V. A. Rogov, E. Yu. Gerasimov and O. A. Bulavchenko
Materials 2022, 15(21), 7553; https://0-doi-org.brum.beds.ac.uk/10.3390/ma15217553 - 27 Oct 2022
Cited by 5 | Viewed by 1424
Abstract
MnOx-CeO2, MnOx-ZrO2, MnOx-ZrO2-CeO2 oxides with the Mn/(Zr + Ce + Mn) molar ratio of 0.3 were synthesized by coprecipitation method followed by calcination in the temperature range of 400–800 °C [...] Read more.
MnOx-CeO2, MnOx-ZrO2, MnOx-ZrO2-CeO2 oxides with the Mn/(Zr + Ce + Mn) molar ratio of 0.3 were synthesized by coprecipitation method followed by calcination in the temperature range of 400–800 °C and characterized by XRD, N2 adsorption, TPR, TEM, and EPR. The catalytic activity was tested in the CO oxidation reaction. It was found that MnOx-CeO2, MnOx-ZrO2-CeO2, MnOx-ZrO2 catalysts, calcined at 400–500 °C, 650–700 °C and 500–650 °C, respectively, show the highest catalytic activity in the reaction of CO oxidation. According to XRD and TEM results, thermal stability of catalysts is determined by the temperature of decomposition of the solid solution Mnx(Ce,Zr)1−xO2. The TPR-H2 and EPR methods showed that the high activity in CO oxidation correlates with the content of easily reduced fine MnOx particles in the samples and the presence of paramagnetic defects in the form of oxygen vacancies. The maximum activity for each series of catalysts is associated with the start of solid solution decomposition. Formation of active phase shifts to the high-temperature region with the addition of zirconium to the MnOx-CeO2 catalyst. Full article
(This article belongs to the Special Issue Advanced Materials in Catalysis and Adsorption)
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15 pages, 19911 KiB  
Article
Porous Co-Pt Nanoalloys for Production of Carbon Nanofibers and Composites
by Sofya D. Afonnikova, Anton A. Popov, Yury I. Bauman, Pavel E. Plyusnin, Ilya V. Mishakov, Mikhail V. Trenikhin, Yury V. Shubin, Aleksey A. Vedyagin and Sergey V. Korenev
Materials 2022, 15(21), 7456; https://0-doi-org.brum.beds.ac.uk/10.3390/ma15217456 - 24 Oct 2022
Cited by 6 | Viewed by 1627
Abstract
The controllable synthesis of carbon nanofibers (CNF) and composites based on CNF (Metals/CNF) is of particular interest. In the present work, the samples of CNF were produced via ethylene decomposition over Co-Pt (0–100 at.% Pt) microdispersed alloys prepared by a reductive thermolysis of [...] Read more.
The controllable synthesis of carbon nanofibers (CNF) and composites based on CNF (Metals/CNF) is of particular interest. In the present work, the samples of CNF were produced via ethylene decomposition over Co-Pt (0–100 at.% Pt) microdispersed alloys prepared by a reductive thermolysis of multicomponent precursors. XRD analysis showed that the crystal structure of alloys in the composition range of 5–35 at.% Pt corresponds to a fcc lattice based on cobalt (Fm-3m), while the CoPt (50 at.% Pt) and CoPt3 (75 at.% Pt) samples are intermetallics with the structure P4/mmm and Pm-3m, respectively. The microstructure of the alloys is represented by agglomerates of polycrystalline particles (50–150 nm) interconnected by the filaments. The impact of Pt content in the Co1−xPtx samples on their activity in CNF production was revealed. The interaction of alloys with ethylene is accompanied by the generation of active particles on which the growth of nanofibers occurs. Plane Co showed low productivity (~5.5 g/gcat), while Pt itself exhibited no activity at all. The addition of 15–25 at.% Pt to cobalt catalyst leads to an increase in activity by 3–5 times. The maximum yield of CNF reached 40 g/gcat for Co0.75Pt0.25 sample. The local composition of the active alloyed particles and the structural features of CNF were explored. Full article
(This article belongs to the Special Issue Advanced Materials in Catalysis and Adsorption)
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14 pages, 4992 KiB  
Article
Composite Structured M/Ce0.75Zr0.25O2/Al2O3/FeCrAl (M = Pt, Rh, and Ru) Catalysts for Propane and n-Butane Reforming to Syngas
by Natalia Ruban, Vladimir Rogozhnikov, Sergey Zazhigalov, Andrey Zagoruiko, Vyacheslav Emelyanov, Pavel Snytnikov, Vladimir Sobyanin and Dmitriy Potemkin
Materials 2022, 15(20), 7336; https://0-doi-org.brum.beds.ac.uk/10.3390/ma15207336 - 20 Oct 2022
Cited by 6 | Viewed by 1372
Abstract
Here, we report the preparation, characterization, and performance of reforming propane and n-butane into a syngas of composite structured M/Ce0.75Zr0.25O2/Al2O3/FeCrAl (M = 0.46 wt.% Pt, 0.24 wt.% Rh, and 0.24 wt.% Ru) catalysts. [...] Read more.
Here, we report the preparation, characterization, and performance of reforming propane and n-butane into a syngas of composite structured M/Ce0.75Zr0.25O2/Al2O3/FeCrAl (M = 0.46 wt.% Pt, 0.24 wt.% Rh, and 0.24 wt.% Ru) catalysts. The catalysts are composed of a high-heat-conducting FeCrAl block with preset geometry, with a surface nearly totally covered by θ-Al2O3. Afterwards, a layer of ceria–zirconia mixed oxide was deposited. The formed oxide coating was used as a support for 2–3 nm sized Pt, Rh, or Ru nanoparticles. The performance of the catalysts in propane steam reforming decreased in the order of Rh ≈ Ru > Pt. The reformates obtained in the propane steam reforming over Rh- and Ru/Ce0.75Zr0.25O2/Al2O3/FeCrAl at 600 °C and GHSV = 8300 h−1 contained 65.2 and 62.4 vol.% of H2, respectively, and can be used as a fuel for solid oxide fuel cells. In the oxidative steam reforming of propane at 700 °C and GHSV= 17,000 h−1, the activities of the Rh- and Pt-based catalysts were similar and the compositions of the outlet gas mixtures were quite close to equilibrium in both cases. Increasing the reagent flow rate to 25,600 h−1 showed stability of the Rh/Ce0.75Zr0.25O2/Al2O3/FeCrAl performance, whereas the Pt/Ce0.75Zr0.25O2/Al2O3/FeCrAl activity decreased. A mathematical model considering the velocity field, mass balance, pressure, and temperature distribution, as well as the reaction kinetics, was suggested for the propane steam and oxidative steam reforming over the Pt- and Rh/Ce0.75Zr0.25O2/Al2O3/FeCrAl catalysts. The model well described the experimental results. Full article
(This article belongs to the Special Issue Advanced Materials in Catalysis and Adsorption)
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11 pages, 3725 KiB  
Article
High Throughput Preparation of Ag-Zn Alloy Thin Films for the Electrocatalytic Reduction of CO2 to CO
by Jiameng Sun, Bin Yu, Xuejiao Yan, Jianfeng Wang, Fuquan Tan, Wanfeng Yang, Guanhua Cheng and Zhonghua Zhang
Materials 2022, 15(19), 6892; https://0-doi-org.brum.beds.ac.uk/10.3390/ma15196892 - 04 Oct 2022
Cited by 6 | Viewed by 1577
Abstract
Ag-Zn alloys are identified as highly active and selective electrocatalysts for CO2 reduction reaction (CO2RR), while how the phase composition of the alloy affects the catalytic performances has not been systematically studied yet. In this study, we fabricated a series [...] Read more.
Ag-Zn alloys are identified as highly active and selective electrocatalysts for CO2 reduction reaction (CO2RR), while how the phase composition of the alloy affects the catalytic performances has not been systematically studied yet. In this study, we fabricated a series of Ag-Zn alloy catalysts by magnetron co-sputtering and further explored their activity and selectivity towards CO2 electroreduction in an aqueous KHCO3 electrolyte. The different Ag-Zn alloys involve one or more phases of Ag, AgZn, Ag5Zn8, AgZn3, and Zn. For all the catalysts, CO is the main product, likely due to the weak CO binding energy on the catalyst surface. The Ag5Zn8 and AgZn3 catalysts show a higher CO selectivity than that of pure Zn due to the synergistic effect of Ag and Zn, while the pure Ag catalyst exhibits the highest CO selectivity. Zn alloying improves the catalytic activity and reaction kinetics of CO2RR, and the AgZn3 catalyst shows the highest apparent electrocatalytic activity. This work found that the activity and selectivity of CO2RR are highly dependent on the element concentrations and phase compositions, which is inspiring to explore Ag-Zn alloy catalysts with promising CO2RR properties. Full article
(This article belongs to the Special Issue Advanced Materials in Catalysis and Adsorption)
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22 pages, 4548 KiB  
Article
The Effect of Sibunit Carbon Surface Modification with Diazonium Tosylate Salts of Pd and Pd-Au Catalysts on Furfural Hydrogenation
by Dmitrii German, Ekaterina Kolobova, Ekaterina Pakrieva, Sónia A. C. Carabineiro, Elizaveta Sviridova, Sergey Perevezentsev, Shahram Alijani, Alberto Villa, Laura Prati, Pavel Postnikov, Nina Bogdanchikova and Alexey Pestryakov
Materials 2022, 15(13), 4695; https://0-doi-org.brum.beds.ac.uk/10.3390/ma15134695 - 04 Jul 2022
Cited by 5 | Viewed by 1747
Abstract
Herein, we investigated the effect of the support modification (Sibunit carbon) with diazonium salts of Pd and Pd-Au catalysts on furfural hydrogenation under 5 bars of H2 and 50 °C. To this end, the surface of Sibunit (Cp) was modified with butyl [...] Read more.
Herein, we investigated the effect of the support modification (Sibunit carbon) with diazonium salts of Pd and Pd-Au catalysts on furfural hydrogenation under 5 bars of H2 and 50 °C. To this end, the surface of Sibunit (Cp) was modified with butyl (Cp-Butyl), carboxyl (Cp-COOH) and amino groups (Cp-NH2) using corresponding diazonium salts. The catalysts were synthesized by the sol immobilization method. The catalysts as well as the corresponding supports were characterized by Fourier transform infrared spectroscopy, N2 adsorption-desorption, inductively coupled plasma atomic emission spectroscopy, high resolution transmission electron microscopy, energy dispersive spectroscopy, X-ray diffraction, Hammet indicator method and X-ray photoelectron spectroscopy. The analysis of the results allowed us to determine the crucial influence of surface chemistry on the catalytic behavior of the studied catalysts, especially regarding selectivity. At the same time, the structural, textural, electronic and acid–base properties of the catalysts were practically unaffected. Thus, it can be assumed that the modification of Sibunit with various functional groups leads to changes in the hydrophobic/hydrophilic and/or electrostatic properties of the surface, which influenced the selectivity of the process. Full article
(This article belongs to the Special Issue Advanced Materials in Catalysis and Adsorption)
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13 pages, 3849 KiB  
Article
CVD-Synthesis of N-CNT Using Propane and Ammonia
by Valery Skudin, Tatiana Andreeva, Maria Myachina and Natalia Gavrilova
Materials 2022, 15(6), 2241; https://0-doi-org.brum.beds.ac.uk/10.3390/ma15062241 - 18 Mar 2022
Cited by 7 | Viewed by 1775
Abstract
N-CNT is a promising material for various applications, including catalysis, electronics, etc., whose widespread use is limited by the significant cost of production. CVD-synthesis using a propane–ammonia mixture is one of the cost-effective processes for obtaining carbon nanomaterials. In this work, the CVD-synthesis [...] Read more.
N-CNT is a promising material for various applications, including catalysis, electronics, etc., whose widespread use is limited by the significant cost of production. CVD-synthesis using a propane–ammonia mixture is one of the cost-effective processes for obtaining carbon nanomaterials. In this work, the CVD-synthesis of N-CNT was conducted in a traditional bed reactor using catalyst: (Al0,4Fe0,48Co0,12)2O3 + 3% MoO3. The synthesized material was characterized by XPS spectroscopy, ASAP, TEM and SEM-microscopy. It is shown that the carbon material contains various morphological structures, including multiwalled carbon nanotubes (MWCNT), bamboo-like structures, spherical and irregular sections. The content of structures (bamboo-like and spherical structure) caused by the incorporation of nitrogen into the carbon nanotube structure depends on the synthesis temperature and the ammonia content in the reaction mixture. The optimal conditions for CVD-synthesis were determined: the temperature range (650–700 °C), the composition (C3H8/NH3 = 50/50%) and flow rate of the ammonia-propane mixture (200 mL/min). Full article
(This article belongs to the Special Issue Advanced Materials in Catalysis and Adsorption)
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14 pages, 32737 KiB  
Article
Green Production of Zero-Valent Iron (ZVI) Using Tea-Leaf Extracts for Fenton Degradation of Mixed Rhodamine B and Methyl Orange Dyes
by Diana Rakhmawaty Eddy, Dian Nursyamsiah, Muhamad Diki Permana, Solihudin, Atiek Rostika Noviyanti and Iman Rahayu
Materials 2022, 15(1), 332; https://0-doi-org.brum.beds.ac.uk/10.3390/ma15010332 - 03 Jan 2022
Cited by 9 | Viewed by 2469
Abstract
The danger from the content of dyes produced by textile-industry waste can cause environmental degradation when not appropriately treated. However, existing waste-treatment methods have not been effective in degrading dyes in textile waste. Zero-valent iron (ZVI), which has been widely used for wastewater [...] Read more.
The danger from the content of dyes produced by textile-industry waste can cause environmental degradation when not appropriately treated. However, existing waste-treatment methods have not been effective in degrading dyes in textile waste. Zero-valent iron (ZVI), which has been widely used for wastewater treatment, needs to be developed to acquire effective green production. Tea (Camellia sinensis) leaves contain many polyphenolic compounds used as natural reducing agents. Therefore, this study aims to synthesize ZVI using biological reducing agents from tea-leaf extract and apply the Fenton method to degrade the color mixture of rhodamine B and methyl orange. The results show that the highest polyphenols were obtained from tea extract by heating to 90 °C for 80 min. Furthermore, PSA results show that ZVI had a homogeneous size of iron and tea extract at a volume ratio of 1:3. The SEM-EDS results show that all samples had agglomerated particles. The ZVI 1:1 showed the best results, with a 100% decrease in the color intensity of the dye mixture for 60 min of reaction and a degradation percentage of 100% and 66.47% for rhodamine B and methyl orange from LC-MS analysis, respectively. Finally, the decrease in COD value by ZVI was 92.11%, higher than the 47.36% decrease obtained using Fe(II). Full article
(This article belongs to the Special Issue Advanced Materials in Catalysis and Adsorption)
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21 pages, 3743 KiB  
Article
Modification of Gold Zeolitic Supports for Catalytic Oxidation of Glucose to Gluconic Acid
by Adrian Walkowiak, Joanna Wolska, Anna Wojtaszek-Gurdak, Izabela Sobczak, Lukasz Wolski and Maria Ziolek
Materials 2021, 14(18), 5250; https://0-doi-org.brum.beds.ac.uk/10.3390/ma14185250 - 13 Sep 2021
Cited by 5 | Viewed by 2021
Abstract
Activity of gold supported catalysts strongly depends on the type and composition of support, which determine the size of Au nanoparticles (Au NPs), gold-support interaction influencing gold properties, interaction with the reactants and, in this way, the reaction pathway. The aim of this [...] Read more.
Activity of gold supported catalysts strongly depends on the type and composition of support, which determine the size of Au nanoparticles (Au NPs), gold-support interaction influencing gold properties, interaction with the reactants and, in this way, the reaction pathway. The aim of this study was to use two types of zeolites: the three dimensional HBeta and the layered two-dimensional MCM-36 as supports for gold, and modification of their properties towards the achievement of different properties in oxidation of glucose to gluconic acid with molecular oxygen and hydrogen peroxide. Such an approach allowed establishment of relationships between the activity of gold catalysts and different parameters such as Au NPs size, electronic properties of gold, structure and acidity of the supports. The zeolites were modified with (3-aminopropyl)-trimethoxysilane (APMS), which affected the support features and Au NPs properties. Moreover, the modification of the zeolite lattice with boron was applied to change the strength of the zeolite acidity. All modifications resulted in changes in glucose conversion, while maintaining high selectivity to gluconic acid. The most important findings include the differences in the reaction steps limiting the reaction rate depending on the nature of the oxidant applied (oxygen vs. H2O2), the important role of porosity of the zeolite supports, and accumulation of negative charge on Au NPs in catalytic oxidation of glucose. Full article
(This article belongs to the Special Issue Advanced Materials in Catalysis and Adsorption)
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Review

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33 pages, 19137 KiB  
Review
Recent Advances in Structured Catalytic Materials Development for Conversion of Liquid Hydrocarbons into Synthesis Gas for Fuel Cell Power Generators
by Vladislav Shilov, Dmitriy Potemkin, Vladimir Rogozhnikov and Pavel Snytnikov
Materials 2023, 16(2), 599; https://0-doi-org.brum.beds.ac.uk/10.3390/ma16020599 - 08 Jan 2023
Cited by 6 | Viewed by 1857
Abstract
The paper considers the current state of research and development of composite structured catalysts for the oxidative conversion of liquid hydrocarbons into synthesis gas for fuel cell feeding and gives more detailed information about recent advances in the Boreskov Institute of Catalysis. The [...] Read more.
The paper considers the current state of research and development of composite structured catalysts for the oxidative conversion of liquid hydrocarbons into synthesis gas for fuel cell feeding and gives more detailed information about recent advances in the Boreskov Institute of Catalysis. The main factors affecting the progress of the target reaction and side reactions leading to catalyst deactivation are discussed. The properties of the Rh/Ce0.75Zr0.25O2/Al2O3/FeCrAl composite multifunctional catalyst for the conversion of diesel fuel into synthesis gas are described. The results of the catalyst testing and mathematical modeling of the process of diesel fuel steam–air conversion into synthesis gas are reported. Full article
(This article belongs to the Special Issue Advanced Materials in Catalysis and Adsorption)
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24 pages, 6381 KiB  
Review
Removal of Pharmaceuticals and Personal Care Products (PPCPs) by Free Radicals in Advanced Oxidation Processes
by Jiao Jiao, Yihua Li, Qi Song, Liujin Wang, Tianlie Luo, Changfei Gao, Lifen Liu and Shengtao Yang
Materials 2022, 15(22), 8152; https://0-doi-org.brum.beds.ac.uk/10.3390/ma15228152 - 17 Nov 2022
Cited by 11 | Viewed by 2492
Abstract
As emerging pollutants, pharmaceutical and personal care products (PPCPs) have received extensive attention due to their high detection frequency (with concentrations ranging from ng/L to μg/L) and potential risk to aqueous environments and human health. Advanced oxidation processes (AOPs) are effective techniques for [...] Read more.
As emerging pollutants, pharmaceutical and personal care products (PPCPs) have received extensive attention due to their high detection frequency (with concentrations ranging from ng/L to μg/L) and potential risk to aqueous environments and human health. Advanced oxidation processes (AOPs) are effective techniques for the removal of PPCPs from water environments. In AOPs, different types of free radicals (HO·, SO4·, O2·, etc.) are generated to decompose PPCPs into non-toxic and small-molecule compounds, finally leading to the decomposition of PPCPs. This review systematically summarizes the features of various AOPs and the removal of PPCPs by different free radicals. The operation conditions and comprehensive performance of different types of free radicals are summarized, and the reaction mechanisms are further revealed. This review will provide a quick understanding of AOPs for later researchers. Full article
(This article belongs to the Special Issue Advanced Materials in Catalysis and Adsorption)
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