Engineering Materials for Catalysis

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

Deadline for manuscript submissions: closed (20 October 2021) | Viewed by 26952

Special Issue Editors

Department of Inorganic Chemistry and Technology, National Institute of Chemistry, Hajdrihova 19, SI-1001 Ljubljana, Slovenia
Interests: heterogeneous catalysis; environmental catalysis; reaction kinetics and mechanisms; synthesis and characterization of catalysts; process development and intensification
Special Issues, Collections and Topics in MDPI journals
Department of Inorganic Chemistry and Technology, National Institute of Chemistry, Hajdrihova 19, SI-1001 Ljubljana, Slovenia
Interests: heterogeneous catalysis; design and development of catalysts; structure–property–performance relationships; environmental and energy technologies
TU Wien, Institute of Materials Chemistry, Getreidemarkt 9/BC/165, Vienna AT-1060, Austria
Interests: surface science; model and applied heterogeneous catalysis; environmental catalysis; in situ/operando spectroscopy and microscopy; synchrotron methods

Special Issue Information

Dear colleagues,

Catalysis is a key enabling technology for achieving efficient, economic, and more sustainable utilization of resources. It provides lower energy processes, reduced waste and pollution, as well as improved selectivity in producing added-value products. About 90 % of all chemical processes use catalysts. Heterogeneous catalysts are already a key component in many processes, from petrochemical conversions to catalytic converters, and enable significant benefits such as catalyst/product separation, reuse, and recyclability. As the world moves towards more sustainable technologies and feedstocks to ensure a cleaner future, heterogeneous catalysts will definitely play an even bigger role. This opens the door to the engineering of novel, next-generation multifunctional catalysts, or even requires looking to the past to redesign more traditional catalysts to meet new challenges. In this regard, designing advanced materials at the atomic scale, an understanding of structure–activity and structure–selectivity relationships, and multiscale modelling aspects are of significant importance.

This Special Issue will feature selected contributions presented at the 2020 Summer School of the European Federation of Catalysis Societies (EFCATS, https://skd2020.chem-soc.si/en/2020-efcats-summer-school/), entitled “Engineering Materials for Catalysis” and held from 15–19 September, 2020 in Grand Hotel Bernardin Convention Center, Portorož-Portorose, Slovenia, but is also open to general contributions from the catalysis community. Articles will particularly encompass the following topics: (i) synthesis and characterization of heterogeneous catalysts, (ii) in situ and operando studies, (iii) synchrotron studies, (iv) modelling and multiscale modelling, (v) applications in photocatalysis, (vi) applications in electrocatalysis, and (vii) catalysis in industry.

Prof. Dr. Albin Pintar
Prof. Dr. Nataša Novak Tušar
Prof. Dr. Günther Rupprechter
Guest Editors

Manuscript Submission Information

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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
  • catalyst synthesis and characterization
  • operando studies
  • synchrotron studies
  • structure–property–performance relationships
  • multiscale modelling
  • photocatalysis
  • electrocatalysis
  • industrial applications

Published Papers (8 papers)

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Research

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16 pages, 4803 KiB  
Article
Studies of Clinoptilolite-Rich Zeolitic Tuffs from Different Regions and Their Activity in Photodegradation of Methylene Blue
by Jelena Pavlović, Andraž Šuligoj, Mojca Opresnik, Nataša Novak Tušar, Nataša Zabukovec Logar and Nevenka Rajić
Catalysts 2022, 12(2), 224; https://0-doi-org.brum.beds.ac.uk/10.3390/catal12020224 - 16 Feb 2022
Cited by 5 | Viewed by 1854
Abstract
The present study focuses on clinoptilolite (CLI)-rich natural zeolitic tuffs and their photocatalytic activity in the degradation of cationic organic dyes. CLI from different regions was tested in the photocatalytic degradation of methylene blue (MB) as a model cationic dye. The photocatalytic tests [...] Read more.
The present study focuses on clinoptilolite (CLI)-rich natural zeolitic tuffs and their photocatalytic activity in the degradation of cationic organic dyes. CLI from different regions was tested in the photocatalytic degradation of methylene blue (MB) as a model cationic dye. The photocatalytic tests were performed at room temperature and atmospheric pressure under visible light irradiation. For all the CLI samples, the highest activity was observed at pH = 6. Total MB degradation varied between 70 and 91% (C0 = 10 mg dm–3, 0.2 g dm–3 of photocatalyst, during 300 min). It is suggested that the presence of Fe species in the studied tuffs is responsible for the photocatalytic activity. The activity increases linearly with the Fe content in the tuffs. The MB photodegradation follows the Langmuir–Hinshelwood kinetic model. The recyclability tests showed good stability and efficiency of the photocatalyst. The degradation rate decreased from 91 to 69% during three reaction cycles, indicating a promising potential of natural zeolites in the treatment of textile industry wastewater. Full article
(This article belongs to the Special Issue Engineering Materials for Catalysis)
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15 pages, 2670 KiB  
Article
Defective Grey TiO2 with Minuscule Anatase–Rutile Heterophase Junctions for Hydroxyl Radicals Formation in a Visible Light-Triggered Photocatalysis
by Sanjay Gopal Ullattil, Janez Zavašnik, Ksenija Maver, Matjaž Finšgar, Nataša Novak Tušar and Albin Pintar
Catalysts 2021, 11(12), 1500; https://0-doi-org.brum.beds.ac.uk/10.3390/catal11121500 - 10 Dec 2021
Cited by 2 | Viewed by 2234
Abstract
The novelty of this work was to prepare a series of defect-rich colored TiO2 nanostructures, using a peroxo solvothermal-assisted, high-pressure nitrogenation method. Among these solids, certain TiO2 materials possessed a trace quantity of anatase–rutile heterojunctions, which are beneficial in obtaining high [...] Read more.
The novelty of this work was to prepare a series of defect-rich colored TiO2 nanostructures, using a peroxo solvothermal-assisted, high-pressure nitrogenation method. Among these solids, certain TiO2 materials possessed a trace quantity of anatase–rutile heterojunctions, which are beneficial in obtaining high reaction rates in photocatalytic reactions. In addition, high surface area (above 100 m2/g), even when utilizing a high calcination temperature (500 °C), and absorption of light at higher wavelengths, due to the grey color of the synthesized titania, were observed as an added advantage for photocatalytic hydroxyl radical formation. In this work, we adopted a photoluminescent probe method to monitor the temporal evolution of hydroxyl radicals. As a result, promising hydroxyl radical formations were observed for all the colored samples synthesized at 400 and 500 °C, irrespective of the duration of calcination. Full article
(This article belongs to the Special Issue Engineering Materials for Catalysis)
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17 pages, 23266 KiB  
Article
Elucidating the Influence of the d-Band Center on the Synthesis of Isobutanol
by Johannes Häusler, Joachim Pasel, Friederike Woltmann, Andreas Everwand, Maria Meledina, Helen Valencia, Marta Lipińska-Chwałek, Joachim Mayer and Ralf Peters
Catalysts 2021, 11(3), 406; https://0-doi-org.brum.beds.ac.uk/10.3390/catal11030406 - 23 Mar 2021
Cited by 1 | Viewed by 2932
Abstract
As the search for carbon-efficient synthesis pathways for green alternatives to fossil fuels continues, an expanding class of catalysts have been developed for the upgrading of lower alcohols. Understanding of the acid base functionalities has greatly influenced the search for new materials, but [...] Read more.
As the search for carbon-efficient synthesis pathways for green alternatives to fossil fuels continues, an expanding class of catalysts have been developed for the upgrading of lower alcohols. Understanding of the acid base functionalities has greatly influenced the search for new materials, but the influence of the metal used in catalysts cannot be explained in a broader sense. We address this herein and correlate our findings with the most fundamental understanding of chemistry to date by applying it to d-band theory as part of an experimental investigation. The commercial catalysts of Pt, Rh, Ru, Cu, Pd, and Ir on carbon as a support have been characterized by means of SEM, EDX-mapping, STEM, XRD, N2-physisorption, and H2-chemisorption. Their catalytic activity has been established by means of c-methylation of ethanol with methanol. For all catalysts, the TOF with respect to i-butanol was examined. The Pt/C reached the highest TOF with a selectivity towards i-butanol of 89%. The trend for the TOFs could be well correlated with the d-band centers of the metal, which formed a volcano curve. Therefore, this study is another step towards the rationalization of catalyst design for the upgrading of alcohols into carbon-neutral fuels or chemical feedstock. Full article
(This article belongs to the Special Issue Engineering Materials for Catalysis)
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23 pages, 5609 KiB  
Article
Infrared Thermography as an Operando Tool for the Analysis of Catalytic Processes: How to Use it?
by Robin Mutschler and Emanuele Moioli
Catalysts 2021, 11(3), 311; https://0-doi-org.brum.beds.ac.uk/10.3390/catal11030311 - 26 Feb 2021
Viewed by 2076
Abstract
Infrared (IR) thermography is a powerful tool to measure temperature with high space and time resolution. A particularly interesting application of this technology is in the field of catalysis, where the method can provide new insights into dynamic surface reactions. This paper presents [...] Read more.
Infrared (IR) thermography is a powerful tool to measure temperature with high space and time resolution. A particularly interesting application of this technology is in the field of catalysis, where the method can provide new insights into dynamic surface reactions. This paper presents guidelines for the development of a reactor cell that can aid in the efficient exploitation of infrared thermography for the investigation of catalytic and other surface reactions. Firstly, the necessary properties of the catalytic reactor are described. Secondly, we analyze the requirements towards the catalytic system to be directly observable by IR thermography. This includes the need for a catalyst that provides a sufficiently high heat production (or absorption) rate. To achieve true operando investigation conditions, some dedicated equipment must be developed. Here, we provide the guidelines to assemble a chemical reactor with an IR transmitting window through which the reaction can be studied with the infrared camera along with other best practice tips to achieve results. Furthermore, we present selected examples of catalytic reactions that can be monitored by IR thermography, showing the potential of the technology in revealing transient and steady state chemical phenomena. Full article
(This article belongs to the Special Issue Engineering Materials for Catalysis)
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26 pages, 9578 KiB  
Article
Influence of Alumina Precursor Properties on Cu-Fe Alumina Supported Catalysts for Total Toluene Oxidation as a Model Volatile Organic Air Pollutant
by Tadej Žumbar, Alenka Ristić, Goran Dražić, Hristina Lazarova, Janez Volavšek, Albin Pintar, Nataša Zabukovec Logar and Nataša Novak Tušar
Catalysts 2021, 11(2), 252; https://0-doi-org.brum.beds.ac.uk/10.3390/catal11020252 - 13 Feb 2021
Cited by 6 | Viewed by 2774
Abstract
The structure–property relationship of catalytic supports for the deposition of redox-active transition metals is of great importance for improving the catalytic efficiency and reusability of the catalysts. In this work, the role of alumina support precursors of Cu-Fe/Al2O3 catalysts used [...] Read more.
The structure–property relationship of catalytic supports for the deposition of redox-active transition metals is of great importance for improving the catalytic efficiency and reusability of the catalysts. In this work, the role of alumina support precursors of Cu-Fe/Al2O3 catalysts used for the total oxidation of toluene as a model volatile organic air pollutant is elucidated. Surface characterization of the catalysts revealed that the surface area, pore volume and acid site concentration of the alumina supports are important but not the determining factors for the catalytic activity of the studied catalysts for this type of reaction. The determining factors are the structural order of the support precursor, the homogeneous distribution of the catalytic sites and reducibility, which were elucidated by XRD, NMR, TEM and temperature programed reduction (TPR). Cu–Fe/Al2O3 prepared from bayerite and pseudoboehmite as highly ordered precursors showed better catalytic performance compared to Cu-Fe/Al2O3 derived from the amorphous alumina precursor and dawsonite. Homogeneous distribution of FexOy and CuOx with defined Cu/Fe molar ratio on the Al2O3 support is required for the efficient catalytic performance of the material. The study showed a beneficial effect of low iron concentration introduced into the alumina precursor during the alumina support synthesis procedure, which resulted in a homogeneous metal oxide distribution on the support. Full article
(This article belongs to the Special Issue Engineering Materials for Catalysis)
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18 pages, 5172 KiB  
Article
The Effect of Shape-Controlled Pt and Pd Nanoparticles on Selective Catalytic Hydrodechlorination of Trichloroethylene
by Oğuz Yunus Sarıbıyık, Christian Weilach, Selahattin Serin and Günther Rupprechter
Catalysts 2020, 10(11), 1314; https://0-doi-org.brum.beds.ac.uk/10.3390/catal10111314 - 13 Nov 2020
Cited by 12 | Viewed by 6540
Abstract
Tailoring the shape of nanoscale materials enables obtaining morphology-controlled surfaces exhibiting specific interactions with reactants during catalytic reactions. The specifics of nanoparticle surfaces control the catalytic performance, i.e., activity and selectivity. In this study, shape-controlled Platinum (Pt) and Palladium (Pd) nanoparticles with distinct [...] Read more.
Tailoring the shape of nanoscale materials enables obtaining morphology-controlled surfaces exhibiting specific interactions with reactants during catalytic reactions. The specifics of nanoparticle surfaces control the catalytic performance, i.e., activity and selectivity. In this study, shape-controlled Platinum (Pt) and Palladium (Pd) nanoparticles with distinct morphology were produced, i.e., cubes and cuboctahedra for Pt and spheres and polyhedra/multiple-twins for Pd, with (100), (111 + 100), curved/stepped and (111) facets, respectively. These particles with well-tuned surfaces were subsequently deposited on a Zirconium oxide (ZrO2) support. The morphological characteristics of the particles were determined by high resolution transmission electron microscopy (HR-TEM) and X-ray diffraction (XRD), while their adsorption properties were investigated by Fourier transform infrared spectroscopy (FTIR) of CO adsorbed at room temperature. The effect of the nanoparticle shape and surface structure on the catalytic performance in hydrodechlorination (HDCl) of trichloroethylene (TCE) was examined. The results show that nanoparticles with different surface orientations can be employed to affect selectivity, with polyhedral and multiply-twinned Pd exhibiting the best ethylene selectivity. Full article
(This article belongs to the Special Issue Engineering Materials for Catalysis)
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15 pages, 3281 KiB  
Article
Management of γ-Alumina with High-Efficient {111} External Surfaces for HDS Reactions
by Yingrui Xu, Shunqin Liang, Limin Sun, Xiaoli Hu, Yuqi Zhang, Weikun Lai, Xiaodong Yi and Weiping Fang
Catalysts 2020, 10(11), 1254; https://0-doi-org.brum.beds.ac.uk/10.3390/catal10111254 - 30 Oct 2020
Cited by 1 | Viewed by 2145
Abstract
A series of γ-alumina samples with different exposure ratio of {111} facet were synthesized by an efficient hydrothermal method via adjusting the pH value of the gel precursor. The nanorod alumina supported catalyst with the highest exposure of {111} facet exhibited the best [...] Read more.
A series of γ-alumina samples with different exposure ratio of {111} facet were synthesized by an efficient hydrothermal method via adjusting the pH value of the gel precursor. The nanorod alumina supported catalyst with the highest exposure of {111} facet exhibited the best hydrodesulfurization (HDS) activities of both thiophene and dibenzothiophene (DBT). Characterization of the sulfided NiMo/Al2O3 catalyst with preferential exposure of {111} facet showed that the MoS2 nano slabs were inclined to distribute in the direction along the edges of alumina nanocrystal in reduced stacking layers. The selective exposure of {111} facet played a decisive role in obtaining alumina-supported HDS catalysts with improved intrinsic activity. This work helps to better understand the relationship between catalytic properties and varied support surfaces, which demonstrate a proper design of the catalyst support morphology on the facet-level. Full article
(This article belongs to the Special Issue Engineering Materials for Catalysis)
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Review

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20 pages, 20276 KiB  
Review
Chemical and Laser Ablation Synthesis of Monometallic and Bimetallic Ni-Based Nanoparticles
by Niusha Lasemi and Günther Rupprechter
Catalysts 2020, 10(12), 1453; https://0-doi-org.brum.beds.ac.uk/10.3390/catal10121453 - 11 Dec 2020
Cited by 17 | Viewed by 4453
Abstract
The catalytic properties of nanoparticles depend on their size, shape and surface/defect structure, with the entire catalyst performance being governed by the corresponding distributions. Herein, we present two routes of mono- and bimetallic nanoparticle synthesis that enable control of the structural parameters, i.e., [...] Read more.
The catalytic properties of nanoparticles depend on their size, shape and surface/defect structure, with the entire catalyst performance being governed by the corresponding distributions. Herein, we present two routes of mono- and bimetallic nanoparticle synthesis that enable control of the structural parameters, i.e., wet-chemical synthesis and laser ablation in liquid-phase. The latter is particularly suited to create defect-rich nanoparticles. Impregnation routes were applied to prepare Ni and NiCu nanoparticles, whereas nano- and femtosecond laser ablation in liquid-phase were employed to prepare Ni and NiAu nanoparticles. The effects of the Ni:Cu ratio in impregnation and of laser fluence and liquid-medium on laser ablation are discussed. The atomic structure and (surface) composition of the nanoparticles were characterized by electron microscopic (BF-TEM, DF-TEM, HRTEM) and spectroscopic/diffraction techniques (EDX, SAED, XPS, IR), complemented by theory (DFT). The chemically synthesized bimetallic NiCu nanoparticles initially had Cu-rich surfaces, which changed to Ni-rich upon reaction. For laser ablation, depending on conditions (fluence, type of liquid), highly defective, ordered, or core/shell-like nanoparticles were produced. The case studies highlight the specific benefits of each preparation method for catalyst synthesis and discuss the potential of nanoparticles produced by pulsed laser ablation for catalytic applications. Full article
(This article belongs to the Special Issue Engineering Materials for Catalysis)
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