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Contemporary Solutions for Advanced Catalytic Materials with a High Impact on Society

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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 (1 August 2022) | Viewed by 27972

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Prof. Dr. Simona M. Coman

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Department of Inorganic Chemistry, Organic Chemistry, Biochemistry and Catalysis, Faculty of Chemistry, University of Bucharest, Bucharest, Romania
Interests: heterogeneous catalysis; asymmetric catalysis; organocatalysis; green chemistry; biomass valorization
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Dr. Madalina Tudorache

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Department of Organic Chemistry, Biochemistry and Catalysis, Faculty of Chemistry, University of Bucharest, Bd. Regina Elisabeta no. 4-12, 030018 Bucharest, Romania
Interests: application of enzymes for the environment monitorization, clinical analysis and industrial synthesis of added-value products; enzyme/whole cell catalysis; enzyme immobilization; biomass valorization
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Dr. Elisabeth Egholm Jacobsen

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Department of Chemistry, Norwegian University of Science and Technology, Høgskoleringen 5, 7491 Trondheim, Norway
Interests: biocatalysis; enantiopure biologically active compounds; chiral chromatography; natural product chemistry
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Special Issue Information

Dear Colleagues,

The progress of contemporary society is basely related to the area of advanced materials, using novel and sophisticated designs and involving high-performance technology and material synthesis. Most advanced materials are designed for catalytic applications to satisfy the continuous requirements of our modern life, which is increasingly dependent on the catalysis. Therefore, advanced catalytic materials offer new solutions for healthcare (pharmaceuticals and therapeutics), energy (petrochemicals), new materials (polymers), transport (catalytic convertors), and the environment (water/air quality, renewable and bioproduced materials).

The main aim of this Special Issue is to highlight the contribution of advanced catalytic materials in the evolution of contemporary society, delivering practical and useful solutions with a positive societal, economic, and environmental impact. Therefore, several aspects will be considered related to the synthesis, characterization, and applications of the advanced catalytic materials. Original research papers and reviews providing new insights into the area of advanced catalytic materials are welcome.

Prof. Dr. Simona M. Coman
Dr. Madalina Tudorache
Dr. Elisabeth Egholm Jacobsen
Guest Editors

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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 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

Advanced catalytic materials
Nanomaterials with catalytic properties
Catalytic materials from biomass
Novel approaches for the synthesis of advanced catalytic materials
New technologies for the characterization of advanced catalytic materials
Green catalysis
Biocatalysis
Photocatalysis
Environmental catalysis

Published Papers (10 papers)

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Research

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18 pages, 5777 KiB

Open AccessArticle

Catalytic Hydrotreatment of Humins Waste over Bifunctional Pd-Based Zeolite Catalysts

by Magdi El Fergani, Natalia Candu, Iunia Podolean, Bogdan Cojocaru, Adela Nicolaev, Cristian M. Teodorescu, Madalina Tudorache, Vasile I. Parvulescu and Simona M. Coman

Catalysts 2022, 12(10), 1202; https://doi.org/10.3390/catal12101202 - 09 Oct 2022

Cited by 1 | Viewed by 1755

Abstract

The catalytic hydrotreatment of humins, the solid byproduct produced from the conversion of C6 sugars (glucose, fructose) to 5-hydroxymethylfurfural (HMF), using supported Pd@zeolite (Beta, Y, and USY) catalysts with different amounts of Pd (i.e., 0.5, 1.0 and 1.5 wt%) was investigated under molecular hydrogen pressure. The highest conversion of humins (52.0%) was obtained on 1.5Pd@USY catalyst while the highest amount of humins oil (27.3%) was obtained in the presence of the 1Pd@Beta zeolite sample, at P_H2 = 30 bars and T = 250 °C. The major compounds in the humins oil evidenced by GC-MS are alcohols, organic acids, ethers, and alkyl-phenolics. However, although all these classes of compounds are obtained regardless of the nature of the catalyst used, the composition of the mixture differs from one catalyst to another. Furanic compounds were not identified in the reaction products. A possible explanation may be related to their high reactivity under the reaction conditions, in the presence of the Pd-based catalysts these compounds lead to alkyl phenolics, important intermediates in the petrochemical industry. Full article

(This article belongs to the Special Issue Contemporary Solutions for Advanced Catalytic Materials with a High Impact on Society)

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13 pages, 2438 KiB

Open AccessFeature PaperArticle

Use of Photocatalytically Active Supramolecular Organic–Inorganic Magnetic Composites as Efficient Route to Remove β-Lactam Antibiotics from Water

by Sabina G. Ion, Octavian D. Pavel, Nicolae Guzo, Madalina Tudorache, Simona M. Coman, Vasile I. Parvulescu, Bogdan Cojocaru and Elisabeth E. Jacobsen

Catalysts 2022, 12(9), 1044; https://doi.org/10.3390/catal12091044 - 14 Sep 2022

Cited by 3 | Viewed by 1884

Abstract

Considerable efforts have been made in recent years to identify an optimal treatment method for the removal of antibiotics from wastewaters. A series of supramolecular organic-inorganic magnetic composites containing Zn-modified MgAl LDHs and Cu-phthalocyanine as photosensitizers were prepared with the aim of removing β-lactam antibiotics from aqueous solutions. The characterization of these materials confirmed the anchorage of Cu-phthalocyanine onto the edges of the LDH lamellae, with a negligible part inserted in the interlayer space. The removal of the β-lactam antibiotics occurred via concerted adsorption and photocatalytic degradation. The efficiency of the composites depended on (i) the LDH: magnetic nanoparticle (MP) ratio, which was strongly correlated with the textural properties of the catalysts, and (ii) the phthalocyanine loading in the final composite. The maximum efficiency was achieved with a removal of ~93% of the antibiotics after 2 h of reaction. Full article

(This article belongs to the Special Issue Contemporary Solutions for Advanced Catalytic Materials with a High Impact on Society)

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12 pages, 1328 KiB

Open AccessArticle

Green Chemo-Enzymatic Protocols for the Synthesis of Enantiopure β-Blockers (S)-Esmolol and (S)-Penbutolol

by Susanne Hansen Troøyen, Lucas Bocquin, Anna Lifen Tennfjord, Kristoffer Klungseth and Elisabeth Egholm Jacobsen

Catalysts 2022, 12(9), 980; https://doi.org/10.3390/catal12090980 - 31 Aug 2022

Cited by 3 | Viewed by 1441

Abstract

The β-blocker (S)-esmolol, has been synthesized in 97% enantiomeric excess and 26% total yield in a four-step synthesis, with a transesterification step of the racemic chlorohydrin methyl 3-(4-(3-chloro-2-hydroxypropoxy)phenyl)propanoate, catalysed by lipase B from Candida antarctica from Syncozymes, Shanghai, China. The β-blocker (S)-penbutolol, has been synthesized in 99% enantiomeric excess and in 22% total yield. The transesterification step of the racemic chlorohydrin 1-chloro-3-(2-cyclopentylphenoxy)propan-2-ol was catalyzed by the same lipase as used for the esmolol building block. We have used different bases for the deprotonation step of the starting phenols, and vinyl butanoate as the acyl donor in the transesterification reactions. The reaction times for the kinetic resolution steps catalysed by the lipase varied from 23 to 48 h, and were run at 30–38 °C. Specific rotation values confirmed the absolute configuration of the enantiopure drugs, however, an earlier report of the specific rotation value of (S)-esmolol is not consistent with our measured specific rotation values, and we here claim that our data are correct. Compared to the previously reported syntheses of these two enantiopure drugs, we have replaced toluene or dichloromethane with acetonitrile, and replaced the flammable acetyl chloride with lithium chloride. We have also reduced the amount of epichlorohydrin and bases, and identified dimeric byproducts in order to obtain higher yields. Full article

(This article belongs to the Special Issue Contemporary Solutions for Advanced Catalytic Materials with a High Impact on Society)

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17 pages, 7394 KiB

Open AccessArticle

ZnO/CQDs Nanocomposites for Visible Light Photodegradation of Organic Pollutants

by Elena E. Toma, Giuseppe Stoian, Bogdan Cojocaru, Vasile I. Parvulescu and Simona M. Coman

Catalysts 2022, 12(9), 952; https://doi.org/10.3390/catal12090952 - 26 Aug 2022

Cited by 9 | Viewed by 2180

Abstract

Currently, carbon quantum dots (CQDs) have been widely investigated as an enhancing photocatalytic component of various nanocomposites. In this study, hetero-structures containing carbon quantum dots (CQDs) associated to zinc oxide were prepared following two one-pot procedures: (i) a hydrothermal approach in which commercial ZnO was used as carrier for CQDs; and (ii) an approach in which the ZnO/CQDs samples were produced in situ by adding zinc acetate to an aqueous suspension of CQDs. CQDs were prepared in advance by a low-temperature hydrothermal (LHT) treatment of useless humins wastes produced by the glucose dehydration in an acidic medium. These samples were characterized by several techniques such asadsorption-desorption isotherms of liquid nitrogen at 77K, X-ray diffraction (XRD), infrared diffuse reflectance with Fourier transform (DRIFT) and UV-vis spectroscopy. The photocatalytic behavior of these materials was investigated in the degradation of methylene blue (MB). The obtained results revealed electronic interactions between CQDs and ZnO which have as an effect an enhancement of the charge separation and diminution of the charge recombination. In accordance, a correlation between the photocatalytic activity and the intrinsic properties of ZnO/CQDs has been evidenced. The highest photocatalytic activity corresponded to the heterostructure containing highly dispersed narrow sized CQDs onto ZnO. Under visible light irradiation and after 180 min of irradiation, MB was degraded by as much as 97.6%. Full article

(This article belongs to the Special Issue Contemporary Solutions for Advanced Catalytic Materials with a High Impact on Society)

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13 pages, 4243 KiB

Open AccessArticle

Methane Hydrate Formation in Hollow ZIF-8 Nanoparticles for Improved Methane Storage Capacity

by Chong Chen, Yun Li and Jilin Cao

Catalysts 2022, 12(5), 485; https://doi.org/10.3390/catal12050485 - 26 Apr 2022

Cited by 5 | Viewed by 2160

Abstract

Methane hydrate has been extensively studied as a potential medium for natural gas storage and transportation. Due to their high specific surface area, tunable porous structure, and surface chemistry, metal–organic frameworks are ideal materials to exhibit the catalytic effect for the formation process of gas hydrate. In this paper, hollow ZIF-8 nanoparticles are synthesized using the hard template method. The synthesized hollow ZIF-8 nanoparticles are used in the adsorption and methane hydrate formation process. The effect of pre-adsorbed water mass in hollow ZIF-8 nanoparticles on methane storage capacity and the hydrate formation rate is investigated. The storage capacity of methane on wet, hollow ZIF-8 is augmented with an increase in the mass ratio of pre-adsorbed water and dry, hollow ZIF-8 (R_W), and the maximum adsorption capacity of methane on hollow ZIF-8 with a R_W of 1.2 can reach 20.72 mmol/g at 275 K and 8.57 MPa. With the decrease in R_W, the wet, hollow ZIF-8 exhibits a shortened induction time and an accelerated growth rate. The formation of methane hydrate on hollow ZIF-8 is further demonstrated with the enthalpy of the generation reaction. This work provides a promising alternative material for methane storage. Full article

(This article belongs to the Special Issue Contemporary Solutions for Advanced Catalytic Materials with a High Impact on Society)

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15 pages, 4034 KiB

Open AccessArticle

Modification of Silica Xerogels with Polydopamine for Lipase B from Candida antarctica Immobilization

by Honghai Wang, Wenda Yue, Shuling Zhang, Yu Zhang, Chunli Li and Weiyi Su

Catalysts 2021, 11(12), 1463; https://doi.org/10.3390/catal11121463 - 30 Nov 2021

Cited by 3 | Viewed by 1479

Abstract

Silica xerogels have been proposed as a potential support to immobilize enzymes. Improving xerogels’ interactions with such enzymes and their mechanical strengths is critical to their practical applications. Herein, based on the mussel-inspired chemistry, we demonstrated a simple and highly effective strategy for stabilizing enzymes embedded inside silica xerogels by a polydopamine (PDA) coating through in-situ polymerization. The modified silica xerogels were characterized by scanning and transmission electron microscopy, Fourier tranform infrared spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy and pore structure analyses. When the PDA-modified silica xerogels were used to immobilize enzymes of Candida antarctica lipase B (CALB), they exhibited a high loading ability of 45.6 mg/g_support, which was higher than that of immobilized CALB in silica xerogels (28.5 mg/g_support). The immobilized CALB of the PDA-modified silica xerogels retained 71.4% of their initial activities after 90 days of storage, whereas the free CALB retained only 30.2%. Moreover, compared with the immobilization of enzymes in silica xerogels, the mechanical properties, thermal stability and reusability of enzymes immobilized in PDA-modified silica xerogels were also improved significantly. These advantages indicate that the new hybrid material can be used as a low-cost and effective immobilized-enzyme support. Full article

(This article belongs to the Special Issue Contemporary Solutions for Advanced Catalytic Materials with a High Impact on Society)

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14 pages, 2745 KiB

Open AccessFeature PaperArticle

Cold-Active Lipase-Based Biocatalysts for Silymarin Valorization through Biocatalytic Acylation of Silybin

by Giulia Roxana Gheorghita, Victoria Ioana Paun, Simona Neagu, Gabriel-Mihai Maria, Madalin Enache, Cristina Purcarea, Vasile I. Parvulescu and Madalina Tudorache

Catalysts 2021, 11(11), 1390; https://doi.org/10.3390/catal11111390 - 17 Nov 2021

Viewed by 1775

Abstract

Extremophilic biocatalysts represent an enhanced solution in various industrial applications. Integrating enzymes with high catalytic potential at low temperatures into production schemes such as cold-pressed silymarin processing not only brings value to the silymarin recovery from biomass residues, but also improves its solubility properties for biocatalytic modification. Therefore, a cold-active lipase-mediated biocatalytic system has been developed for silybin acylation with methyl fatty acid esters based on the extracellular protein fractions produced by the psychrophilic bacterial strain Psychrobacter SC65A.3 isolated from Scarisoara Ice Cave (Romania). The extracellular production of the lipase fraction was enhanced by 1% olive-oil-enriched culture media. Through multiple immobilization approaches of the cold-active putative lipases (using carbodiimide, aldehyde-hydrazine, or glutaraldehyde coupling), bio-composites (S1–5) with similar or even higher catalytic activity under cold-active conditions (25 °C) have been synthesized by covalent attachment to nano-/micro-sized magnetic or polymeric resin beads. Characterization methods (e.g., FTIR DRIFT, SEM, enzyme activity) strengthen the biocatalysts’ settlement and potential. Thus, the developed immobilized biocatalysts exhibited between 80 and 128% recovery of the catalytic activity for protein loading in the range 90–99% and this led to an immobilization yield up to 89%. The biocatalytic acylation performance reached a maximum of 67% silybin conversion with methyl decanoate acylating agent and nano-support immobilized lipase biocatalyst. Full article

(This article belongs to the Special Issue Contemporary Solutions for Advanced Catalytic Materials with a High Impact on Society)

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15 pages, 1892 KiB

Open AccessFeature PaperArticle

Lipase Catalyzed Synthesis of Enantiopure Precursors and Derivatives for β-Blockers Practolol, Pindolol and Carteolol

by Morten Andre Gundersen, Guro Buaas Austli, Sigrid Sløgedal Løvland, Mari Bergan Hansen, Mari Rødseth and Elisabeth Egholm Jacobsen

Catalysts 2021, 11(4), 503; https://doi.org/10.3390/catal11040503 - 16 Apr 2021

Cited by 9 | Viewed by 2899

Abstract

Sustainable methods for producing enantiopure drugs have been developed. Chlorohydrins as building blocks for several β-blockers have been synthesized in high enantiomeric purity by chemo-enzymatic methods. The yield of the chlorohydrins increased by the use of catalytic amount of base. The reason for this was found to be the reduced formation of the dimeric by-products compared to the use of higher concentration of the base. An overall reduction of reagents and reaction time was also obtained compared to our previously reported data of similar compounds. The enantiomers of the chlorohydrin building blocks were obtained by kinetic resolution of the racemate in transesterification reactions catalyzed by Candida antarctica Lipase B (CALB). Optical rotations confirmed the absolute configuration of the enantiopure drugs. The β-blocker (S)-practolol ((S)-N-(4-(2-hydroxy-3-(isopropylamino)propoxy)phenyl)acetamide) was synthesized with 96% enantiomeric excess (ee) from the chlorohydrin (R)-N-(4-(3-chloro-2 hydroxypropoxy)phenyl)acetamide, which was produced in 97% ee and with 27% yield. Racemic building block 1-((1H-indol-4-yl)oxy)-3-chloropropan-2-ol for the β-blocker pindolol was produced in 53% yield and (R)-1-((1H-indol-4-yl)oxy)-3-chloropropan-2-ol was produced in 92% ee. The chlorohydrin 7-(3-chloro-2-hydroxypropoxy)-3,4-dihydroquinolin-2(1H)-one, a building block for a derivative of carteolol was produced in 77% yield. (R)-7-(3-Chloro-2-hydroxypropoxy)-3,4-dihydroquinolin-2(1H)-one was obtained in 96% ee. The S-enantiomer of this carteolol derivative was produced in 97% ee in 87% yield. Racemic building block 5-(3-chloro-2-hydroxypropoxy)-3,4-dihydroquinolin-2(1H)-one, building block for the drug carteolol, was also produced in 53% yield, with 96% ee of the R-chlorohydrin (R)-5-(3-chloro-2-hydroxypropoxy)-3,4-dihydroquinolin-2(1H)-one. (S)-Carteolol was produced in 96% ee with low yield, which easily can be improved. Full article

(This article belongs to the Special Issue Contemporary Solutions for Advanced Catalytic Materials with a High Impact on Society)

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Review

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15 pages, 967 KiB

Open AccessReview

Properties and Recyclability of Abandoned Fishing Net-Based Plastic Debris

by Anna Kozioł, Kristofer Gunnar Paso and Stanisław Kuciel

Catalysts 2022, 12(9), 948; https://doi.org/10.3390/catal12090948 - 26 Aug 2022

Cited by 7 | Viewed by 7852

Abstract

Plastics in marine environments undergo molecular degradation via biocatalytic and photocatalytic mechanisms. Abandoned, lost, or discarded fishing gear (ALDFG) damages marine and coastal environments as well as plant and animal species. This article reviews ghost fishing, ecological damage from marine plastics, recommended recycling practices and alternative usages of derelict fishing gear. Material mixing techniques are proposed to counteract the effect of biocatalytic and photocatalytic biodegradation within the context of plastic fish net recycling. There is a need for a new and rapid “multidimensional molecular characterization” technology to quantify, at a batch level, the extent of photocatalytic or biocatalytic degradation experienced on each recovered fishing net, comprising molecular weight alteration, chemical functional group polydispersity and contaminant presence. Rapid multidimensional molecular characterization enables optimized conventional material mixing of recovered fishing nets. In this way, economically attractive social return schemes can be introduced for used fishing nets, providing an economic incentive for fishers to return conventional fishing nets for recycling. Full article

(This article belongs to the Special Issue Contemporary Solutions for Advanced Catalytic Materials with a High Impact on Society)

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24 pages, 6450 KiB

Open AccessReview

Recent Progress on Sulfated Nanozirconia as a Solid Acid Catalyst in the Hydrocracking Reaction

by Serly Jolanda Sekewael, Remi Ayu Pratika, Latifah Hauli, Amalia Kurnia Amin, Maisari Utami and Karna Wijaya

Catalysts 2022, 12(2), 191; https://doi.org/10.3390/catal12020191 - 03 Feb 2022

Cited by 19 | Viewed by 3037

Abstract

Zirconia has advantageous thermal stability and acid–base properties. The acidity character of ZrO₂ can be enhanced through the sulfation process forming sulfated zirconia (ZrO₂-SO₄). An acidity test of the catalyst produced proved that the sulfate loading succeeded in increasing the acidity of ZrO₂ as confirmed by the presence of characteristic absorptions of the sulfate group from the FTIR spectra of the catalyst. The ZrO₂-SO₄ catalyst can be further modified with transition metals, such as Platinum (Pt), Chromium (Cr), and Nickel (Ni) to increase catalytic activity and catalyst stability. It was observed that variations in the concentrations of Pt, Cr, and Ni produced a strong influence on the catalytic activity as the acidity and porosity of the catalyst increased with their addition. The activity, selectivity, and catalytic stability tests of Pt/ZrO₂-SO₄, Cr/ZrO₂-SO₄ and Ni/ZrO₂-SO₄ were carried out with their application in the hydrocracking reaction to produce liquid fuel. The percentage of liquid fractions produced using these catalysts were higher than the fraction produced using pure ZrO₂ and ZrO₂-SO₄ catalyst. Full article

(This article belongs to the Special Issue Contemporary Solutions for Advanced Catalytic Materials with a High Impact on Society)

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