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

Deadline for manuscript submissions: closed (31 December 2021) | Viewed by 30650

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Dr. Jose L. Hueso

E-Mail Website1 Website2
Guest Editor

1. Institute of Nanoscience and Materials of Aragon (INMA), Spanish Research Council-University of Zaragoza (CSIC-University of Zaragoza), 50009 Zaragoza, Spain
2. Department of Chemical and Environmental Engineering, University of Zaragoza, 50009 Zaragoza, Spain
3. Centro de Investigación Biomédica en Red (CIBER-BBN), Instituto de Salud Carlos III, 28049 Madrid, Spain
Interests: carbon nanodots; plasmonic photocatalysts; carbon dioxide revalorization; enzyme-like photocatalysts; VOCs oxidation
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Special Issue Information

Dear Colleagues,

The scope of this Special Issue can be defined in the broad context of current search for novel catalyst designs to face multiple research challenges in our XXI century society, which include novel biomedical treatments, environmental protection and remediation, alternative and greener energy sources, process intensification in currently defined processes, etc. Great efforts are being currently made in developing hierarchically ordered materials composed of single or multiple-phase materials (i.e., xerogels, supported catalysts, organic–inorganic composites, MOFs, COFs) that can be self-assembled or structured in previously shaped supports (i.e., monoliths, foams, membranes, 3-D-printed customized shapes, and so on).
Herein, we would like to gather a reference collection of publications describing the most recent efforts carried out in the development of novel synthesis strategies, novel deployment of catalytic materials, novel composite configurations, novel theoretical and practical approaches towards the development of 3-D-printed materials, novel configurations of entangled supports and smart distribution of single-active catalytic materials, novel multilayer configurations for photo, electro-catalytic applications, and any fundamental advances in all kinds of catalytic process. Works related to the development of gels for biological studies (i.e., bioorthogonal catalysis) are also welcome.

Dr. Jose L. Hueso
Guest Editor

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Keywords

Structured catalytic supports
Monoliths
Environmental catalysis
3-D-printed catalytic materials
Self-assembled hierarchical catalysts
Process Intensification
Membranes
Thin Films
Green Energy production
Composites

Published Papers (10 papers)

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Research

9 pages, 1625 KiB

Open AccessCommunication

Development of Monodisperse Mesoporous Microballs Composed of Decahedral Anatase Nanocrystals

by Ying Chang, Jiayi Jiang, Zhishun Wei and Ewa Kowalska

Catalysts 2022, 12(4), 408; https://doi.org/10.3390/catal12040408 - 07 Apr 2022

Viewed by 1438

Abstract

Mesoporous monodisperse microballs of amorphous titania were prepared from solution of absolute ethanol, tetrabutyl titanate (TBOT) and potassium chloride via a sub-zero sol–gel route. The as-obtained microballs were used as the precursor in an alcohothermal (ethanol with a small amount of water) process to synthesize monodisperse mesoporous microballs built of decahedral anatase nanocrystals. FE-SEM observation and XRD analysis have confirmed that the formed decahedral anatase-rich powder retained the original spherical morphology of the precursor. Importantly, a hierarchical structure composed of faceted anatase has been achieved under “green” conditions, i.e., fluorine-free. Additionally, the hysteresis loops (BET results) have confirmed the existence of mesopores. Interestingly, faceted microballs show noticeable photocatalytic activity under UV/vis irradiation for hydrogen generation without any co-catalyst use, reaching almost forty times higher activity than that by famous commercial titania photocatalyst—P25. It has been proposed that enhanced photocatalytic performance is caused by mesoporous structure and co-existence of two kinds of facets, i.e., {001} and {101}, and thus hindered charge carriers’ recombination. Full article

(This article belongs to the Special Issue Structured Materials for Catalytic Applications)

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16 pages, 4927 KiB

Open AccessFeature PaperArticle

Hybrids of Reduced Graphene Oxide Aerogel and CNT for Electrochemical O₂ Reduction

by Javier Hernández-Ferrer, Ana M. Benito, Wolfgang K. Maser and Enrique García-Bordejé

Catalysts 2021, 11(11), 1404; https://doi.org/10.3390/catal11111404 - 20 Nov 2021

Cited by 3 | Viewed by 1861

Abstract

Carbon nanotubes (CNTs), graphene aerogels (GAs), and their hybrid (CNT-GA) prepared by hydrothermal treatment were tested in the electrocatalytic oxygen reduction reaction (ORR). The importance of porous structure derived from the combination of mesoporosity coming from CNTs with macroporosity stemming from GAs was evidenced because the hybrid carbon material exhibited synergistic performance in terms of kinetic current and onset potential. Different electrocatalysts were prepared based on these hybrids doped with nitrogen using different precursors and also supporting Fe nanoparticles. N-doped carbon hybrids showed higher electrocatalytic activity than their undoped counterparts. Nevertheless, both doped and undoped materials provided a mixed two and four electron reduction. On the other hand, the addition of a Fe precursor and phenanthroline to the CNT-GA allowed preparing an N-doped hybrid containing Fe nanoparticles which favored the 4-electron oxygen reduction to water, thus being an excellent candidate as a structured cathode in fuel cells. Full article

(This article belongs to the Special Issue Structured Materials for Catalytic Applications)

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15 pages, 27664 KiB

Open AccessArticle

Bimetallic Zeolite Beta Beads with Hierarchical Porosity as Brønsted-Lewis Solid Acid Catalysts for the Synthesis of Methyl Lactate

by Zahra Asgar Pour, Dina G. Boer, Shun Fang, Zhenchen Tang and Paolo P. Pescarmona

Catalysts 2021, 11(11), 1346; https://doi.org/10.3390/catal11111346 - 09 Nov 2021

Cited by 9 | Viewed by 2201

Abstract

Bimetallic zeolite Beta in bead format and containing Al sites with Brønsted acid behavior and Sn, Zr or Hf sites with Lewis acid character, were prepared using a two-step synthetic route. First, zeolite Beta in the format of macroscopic beads (400 to 840 μm) with hierarchical porosity (micropores accessed through meso- and macropores in the range of 30 to 150 nm) were synthesized by hydrothermal crystallization in the presence of anion-exchange resin beads as hard template and further converted into their H-form. Next, the zeolite beads were partially dealuminated using different concentrations of HNO₃ (i.e., 1.8 or 7.2 M), followed by grafting with one of the above-mentioned metals (Sn, Zr or Hf) to introduce Lewis acid sites. These bimetallic zeolites were tested as heterogeneous catalysts in the conversion of dihydroxyacetone (DHA) to methyl lactate (ML). The Sn-containing zeolite Beta beads treated by 1.8 M HNO₃ and grafted with 27 mmol of SnCl₄ (Sn-deAl-1.8-Beta-B) demonstrated the best catalytic activity among the prepared bimetallic zeolite beads, with 99% selectivity and 90% yield of ML after 6 h at 90 °C. This catalyst was also tested in combination with Au-Pd nanoparticles supported on functionalized carbon nanotubes (CNTs) as multifunctional catalytic system for the conversion of glycerol to ML, achieving 29% conversion of glycerol and 67% selectivity towards ML after 4.5 h at 140 °C under 30 bar air. The catalytic results were rationalized by means of a thorough characterization of the zeolitic beads with a combination of techniques (XRD, N₂-physisorption, SEM, XRF, TEM, UV-vis spectroscopy and pyridine-FT-IR). Full article

(This article belongs to the Special Issue Structured Materials for Catalytic Applications)

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25 pages, 5345 KiB

Open AccessFeature PaperArticle

Hydrodesulfurization of 4,6-Dimethyldibenzothiophene and the Diesel Oil Fraction on NiMo Catalysts Supported over Proton-Exchanged AlMCM-41 and TiMCM-41 Extrudates

by Karolina Jaroszewska, Marek Lewandowski, Kinga Góra-Marek, Jolanta Grzechowiak and Gérald Djéga-Mariadassou

Catalysts 2021, 11(9), 1086; https://doi.org/10.3390/catal11091086 - 09 Sep 2021

Cited by 2 | Viewed by 2331

Abstract

NiMo catalysts supported on mesoporous MCM-41 type materials shaped with binder were tested for activity in the hydrodesulfurization of 4,6-dimethyldibenzothiophene (4,6-DMDBT) and the diesel fuel fraction (0.92 wt% of sulfur). The aim of the investigation was to evaluate the effect of ion exchange with protons of Al- or Ti-substituted MCM-41 mesoporous supports. The subjected catalytic systems were NiMo/HAlMCM-41 and NiMo/HTiMCM-41, and for comparison purposes NiMo/AlMCM-41 and NiMo/TiMCM-41. The samples were characterized by N₂ sorption (at 77 K), XRD, TEM, XPS, SEM and Py–IR. It was found that the functionalization of AlMCM-41 and TiMCM-41 with protons increased the conversion of 4,6-DMDBT and the pseudo-first-order rate constant. Correspondingly, 4,6-DMDBT HDS reactions over the NiMo/HTiMCM-41 catalyst proceeded to a similar extent via hydrogenation and direct desulfurization, whereas over the NiMo/HAlMCM-41 they proceeded mainly via direct desulfurization. Furthermore, the ion-exchanged catalysts displayed two-fold higher efficiency in direct desulfurization than their non-modified counterparts. The NiMo/HTiMCM-41 catalyst exhibited the highest catalytic efficiency in the HDS of 4,6-DMDBT and the diesel oil fraction. The high activity of the NiMo/HTiMCM-41 catalyst is mainly attributed to its appropriate acidity, as well as the metal–support interaction providing both the high dispersion of the active phase and the desirable multilayered stacking morphology of the active phase slabs. Full article

(This article belongs to the Special Issue Structured Materials for Catalytic Applications)

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16 pages, 22401 KiB

Open AccessFeature PaperArticle

PT-BI Co-Deposit Shell on AU Nanoparticle Core: High Performance and Long Durability for Formic Acid Oxidation

by Young Jun Kim, Hyein Lee, Hee-Suk Chung, Youngku Sohn and Choong Kyun Rhee

Catalysts 2021, 11(9), 1049; https://doi.org/10.3390/catal11091049 - 30 Aug 2021

Cited by 2 | Viewed by 1928

Abstract

This work presents the catalysts of Pt-Bi shells on Au nanoparticle cores and Pt overlayers on the Pt-Bi shells toward formic acid oxidation (FAO). Pt and Bi were co-deposited on Au nanoparticles (Au NP) via the irreversible adsorption method using a mixed precursor solution of Pt and Bi ions, and the amount of the co-deposits was controlled with the repetition of the deposition cycle. Rinsing of the co-adsorbed ionic layers of Pt and Bi with a H₂SO₄ solution selectively removed the Bi ions to leave Pt-rich and Bi-lean (<0.4 atomic %) co-deposits on Au NP (Pt-Bi/Au NP), conceptually similar to de-alloying. Additional Pt was deposited over Pt-Bi/Au NPs (Pt/Pt-Bi/Au NPs) to manipulate further the physicochemical properties of Pt-Bi/Au NPs. Transmission electron microscopy revealed the core–shell structures of Pt-Bi/Au NPs and Pt/Pt-Bi/Au NPs, whose shell thickness ranged from roughly four to six atomic layers. Moreover, the low crystallinity of the Pt-containing shells was confirmed with X-ray diffraction. Electrochemical studies showed that the surfaces of Pt-Bi/Au NPs were characterized by low hydrogen adsorption abilities, which increased after the deposition of additional Pt. Durability tests were carried out with 1000 voltammetric cycles between −0.26 and 0.4 V (versus Ag/AgCl) in a solution of 1.0 M HCOOH + 0.1 M H₂SO₄. The initial averaged FAO performance on Pt-Bi/Au NPs and Pt/Pt-Bi/Au NPs (0.11 ± 0.01 A/mg, normalized to the catalyst weight) was higher than that of a commercial Pt nanoparticle catalyst (Pt NP, 0.023 A/mg) by a factor of ~5, mainly due to enhancement of dehydrogenation and suppression of dehydration. The catalytic activity of Pt/Pt-Bi/Au NP (0.04 ± 0.01 A/mg) in the 1000th cycle was greater than that of Pt-Bi/Au NP (0.026 ± 0.003 A/mg) and that of Pt NP (0.006 A/mg). The reason for the higher durability was suggested to be the low mobility of surface Pt atoms on the investigated catalysts. Full article

(This article belongs to the Special Issue Structured Materials for Catalytic Applications)

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27 pages, 9528 KiB

Open AccessArticle

Effect of Textural Properties and Presence of Co-Cation on NH₃-SCR Activity of Cu-Exchanged ZSM-5

by Magdalena Jabłońska, Kinga Góra-Marek, Miha Grilc, Paolo Cleto Bruzzese, David Poppitz, Kamila Pyra, Michael Liebau, Andreas Pöppl, Blaž Likozar and Roger Gläser

Catalysts 2021, 11(7), 843; https://doi.org/10.3390/catal11070843 - 13 Jul 2021

Cited by 15 | Viewed by 3577

Abstract

Comparative studies over micro-/mesoporous Cu-containing zeolites ZSM-5 prepared by top-down treatment involving NaOH, TPAOH or mixture of NaOH/TPAOH (tetrapropylammonium hydroxide) were conducted. The results of the catalytic data revealed the highest activity of the Cu-ZSM-5 catalyst both in the absence and presence of water vapor. The physico-chemical characterization (diffuse reflectance UV-Vis (DR UV-Vis), Fourier transform infrared (FT-IR) spectroscopy, electron paramagnetic resonance (EPR) spectroscopy, temperature-programmed desorption of NO_x (TPD-NO_x), and microkinetic modeling) results indicated that the microporous structure of ZSM-5 effectively stabilized isolated Cu ion monomers. Besides the attempts targeted to the modification of the textural properties of the parent ZSM-5, in the next approach, we studied the effect of the co-presence of sodium and copper cations in the microporous H-ZSM-5. The presence of co-cation promoted the evolution of [Cu–O–Cu]²⁺ dimers that bind NO_x strongly with the desorption energy barrier of least 80 kJ mol⁻¹. Water presence in the gas phase significantly decreases the rate of ammonia oxidation, while the reaction rates and activation energies of NH₃-SCR remain unaffected. Full article

(This article belongs to the Special Issue Structured Materials for Catalytic Applications)

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17 pages, 6034 KiB

Open AccessArticle

Efficient Sorbitol Producing Process through Glucose Hydrogenation Catalyzed by Ru Supported Amino Poly (Styrene-co-Maleic) Polymer (ASMA) Encapsulated on γ-Al₂O₃

by Jing Zhao, Xiaorui Yang, Wei Wang, Jinhua Liang, Yasin Orooji, Chaowen Dai, Xiaomin Fu, Yunsong Yang, Wenlong Xu and Jianliang Zhu

Catalysts 2020, 10(9), 1068; https://doi.org/10.3390/catal10091068 - 17 Sep 2020

Cited by 16 | Viewed by 3944

Abstract

In this work, a core-shell-like sphere ruthenium catalyst, named as 5%Ru/γ-Al₂O₃@ASMA, has been successfully synthesized through impregnating the ruthenium nanoparticles (NPs) on the surface of the amino poly (styrene-co-maleic) polymer (ASMA) encapsulating γ-Al₂O₃ pellet support. The interaction between the Ru cations and the electro-donating polymer shell rich in hydroxyl and amino groups through the coordination bond would guarantee that the Ru NPs can be highly dispersed and firmly embedded on the surface of the support. In addition, the solid sphere γ-Al₂O₃ pellet could serve as the core to support the resulted catalysts applied in the flow process in a trickle bed reactor to promote the productivity. The resulted catalyst 5%Ru/γ-Al₂O₃@ASMA can be applied efficiently in the glucose hydrogenation and presents a steadfast sorbitol yield of almost 90% both in batch reactor and the trickle bed reactor, indicating the potential feasibility of the core-shell-like catalyst in the efficient production of sorbitol. Full article

(This article belongs to the Special Issue Structured Materials for Catalytic Applications)

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9 pages, 1501 KiB

Open AccessCommunication

Bimetallic Metal-Organic Framework Mediated Synthesis of Ni-Co Catalysts for the Dry Reforming of Methane

by Il Son Khan, Adrian Ramirez, Genrikh Shterk, Luis Garzón-Tovar and Jorge Gascon

Catalysts 2020, 10(5), 592; https://doi.org/10.3390/catal10050592 - 25 May 2020

Cited by 19 | Viewed by 4545

Abstract

Dry reforming of methane (DRM) involves the conversion of CO₂ and CH₄, the most important greenhouse gases, into syngas, a stoichiometric mixture of H₂ and CO that can be further processed via Fischer–Tropsch chemistry into a wide variety of products. However, the devolvement of the coke resistant catalyst, especially at high pressures, is still hampering commercial applications. One of the relatively new approaches for the synthesis of metal nanoparticle based catalysts comprises the use of metal-organic frameworks (MOFs) as catalyst precursors. In this work we have explored MOF-74/CPO-27 MOFs as precursors for the synthesis of Ni, Co and bimetallic Ni-Co metal nanoparticles. Our results show that the bimetallic system produced through pyrolysis of a Ni-Co@CMOF-74 precursor displays the best activity at moderate pressures, with stable performance during at least 10 h at 700 °C, 5 bar and 33 L·h⁻¹·g⁻¹. Full article

(This article belongs to the Special Issue Structured Materials for Catalytic Applications)

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11 pages, 2427 KiB

Open AccessArticle

Development of (γ-Al₂O₃-Zeolite Y)/α-Al₂O₃-HPCM Catalyst based on Highly Porous α-Al₂O₃-HPCM Support for Decreasing Oil Viscosity

by Alexey Kirgizov, Gulnaz Valieva, Artem Laskin, Il’dar Il’yasov and Alexander Lamberov

Catalysts 2020, 10(2), 250; https://doi.org/10.3390/catal10020250 - 19 Feb 2020

Cited by 3 | Viewed by 2414

Abstract

Highly porous cellular material (α-Al₂O₃-HPCM) support was synthesized by the template method. Highly porous support was used for the synthesis of the catalyst. A thin secondary layer with 25–30 μ thick γ-Al₂O₃ and zeolite Y was applied on the α-Al₂O₃-HPCM surface ((γ-Al₂O₃ (85%)-zeolite Y (15%))/α-Al₂O₃-HPCM). The catalyst based on the highly porous support was tested in a process of decreasing oil viscosity. The catalyst in the form of cylindrical granules and a thermal process of decreasing oil viscosity without the catalyst were used as the basis for comparison. α-Al₂O₃-HPCM in the catalyst provides low-quantity pores (d < 10 nm) and a quantity of general acid centers compared with the granular catalyst. On the other hand, it shows a more significant oil viscosity decrease (from 2500 to 41 cPs) and a low rate of gas generation (137 mL/h) for the catalyst with highly porous support. A high oil fraction was observed in the presence of the (γ-Al₂O₃-zeolite Y)/α-Al₂O₃-HPCM compared to the granular catalyst. The presence of large transport cells (pores) 1500–2000 μ for the catalyst based on highly porous support allowed a work period four times longer than that of experiment only with temperature without catalysts. Full article

(This article belongs to the Special Issue Structured Materials for Catalytic Applications)

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11 pages, 4314 KiB

Open AccessArticle

Impregnation Protocols on Alumina Beads for Controlling the Preparation of Supported Metal Catalysts

by Alejandra C. Bueno, Maxime Mayer, Matthieu Weber, Mikhael Bechelany, Michaela Klotz and David Farrusseng

Catalysts 2019, 9(7), 577; https://doi.org/10.3390/catal9070577 - 30 Jun 2019

Cited by 7 | Viewed by 5322

Abstract

Whereas the synthesis principles of supported metal catalysts are well documented in the open literature, impregnation protocols on shaped bodies represent sensitive industrial know-how and are, therefore, rarely found. We investigated various synthesis parameters for both wetness (WI) and dry (DI) impregnations to prepare Pd/γ–Al₂O₃ alumina beads. Two kinds of catalysts were achieved: homogeneously dispersed catalysts with no metal gradient across the beads and eggshell catalysts. A combination of optical images, Castaing microprobe analysis, elemental analysis, and TEM made it possible to discriminate between catalysts according to their metal loading, location across the bead diameter, and metal dispersion. Regardless of the macropore structure of the alumina beads, we found that volatile solvents (acetone) were preferred for preparing homogeneous catalysts by WI, whereas the use of a viscous aqueous solution (water/glycerol) in DI resulted in an eggshell-type catalyst. The atomic layer deposition (ALD) method was also investigated as a physical vapor phase deposition method for preparing eggshell catalysts. Representative-shaped catalysts were tested for CO oxidation as a model reaction in order to highlight the differences between catalysts with a homogeneous metal distribution (no metal gradient) and eggshell-type. Full article

(This article belongs to the Special Issue Structured Materials for Catalytic Applications)

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