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Catalysts
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Multifunctional Heterogeneous Catalysis
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Multifunctional Heterogeneous Catalysis

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

Deadline for manuscript submissions: closed (15 June 2020) | Viewed by 15299

Special Issue Editors

Dr. José María Fraile

E-Mail Website
Guest Editor
Instituto de Síntesis Química y Catálisis Homogénea (ISQCH), C.S.I.C.−Universidad de Zaragoza, E-50009 Zaragoza, Spain
Interests: heterogeneous catalysis; green chemistry; biorefinery; renewable raw materials
Prof. Dr. Elísabet Pires

E-Mail Website
Guest Editor
Instituto de Síntesis Química y Catálisis Homogénea (ISQCH), CSIC.−Universidad de Zaragoza, E-50009 Zaragoza, Spain
Interests: heterogeneous catalysis; green solvents; glycerol derivatives; biorefinery

Special Issue Information

Dear Colleagues,

One of the challenges of chemical synthesis, which deals with multistep synthetic routes to complicated molecules, is to improve the sustainability of the processes by simplifying separation and purification procedures. Although the usefulness of heterogeneous catalysis in this regard is undeniable, the development of new catalytic systems with improved efficiency is still necessary. Especially single heterogeneous catalysts with different functionalities or different compatible heterogeneous catalysts are of great interest in terms of carrying out one-pot or sequential tandem processes, without the need for purification of the intermediate products. These systems should make the whole process more cost-effective in terms of materials, time and energy consumption, and hence more sustainable in the context of a greener chemistry. These processes can be of special interest in fields such as the conversion of natural biomass into valuable chemicals or the synthesis of pharmaceuticals, where several reaction steps are usually needed.

This Special Issue will try to gather the most recent works dealing with the development and use of bifunctional heterogeneous catalysts or the application of two (or more) heterogeneous catalysts in one-pot or tandem reactions. It is our pleasure to invite you to contribute an original research paper or a review article for this Special Issue.

Prof. José María Fraile
Prof. Elísabet Pires
Guest Editors

Manuscript Submission Information

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

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

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

Keywords

  • One-pot reactions
  • Cascade reactions
  • Multifunctional heterogeneous catalysts
  • Multicatalyst processes

Published Papers (4 papers)

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Research

11 pages, 2049 KiB  
Article
A Highly Efficient Bifunctional Catalyst CoOx/tri-g-C3N4 for One-Pot Aerobic Oxidation–Knoevenagel Condensation Reaction
by Jiequn Wu, Weiming Hua, Yinghong Yue and Zi Gao
Catalysts 2020, 10(6), 712; https://doi.org/10.3390/catal10060712 - 25 Jun 2020
Cited by 10 | Viewed by 2700
Abstract
A highly efficient bifunctional catalyst of an s-triazine-based carbon-nitride-supported cobalt oxide is developed for the aerobic oxidation–Knoevenagel condensation tandem reaction of benzyl alcohol and malononitrile, whereby 96.4% benzyl alcohol conversion with nearly 100% selectivity towards benzylmalononitrile can be obtained in 6 h at [...] Read more.
A highly efficient bifunctional catalyst of an s-triazine-based carbon-nitride-supported cobalt oxide is developed for the aerobic oxidation–Knoevenagel condensation tandem reaction of benzyl alcohol and malononitrile, whereby 96.4% benzyl alcohol conversion with nearly 100% selectivity towards benzylmalononitrile can be obtained in 6 h at 80 °C. The excellent catalytic performance derives from the high basicity of carbon nitride and strong redox ability of Co species induced by carbon nitride. The catalyst is also quite stable and can be reused without any regeneration treatment, whose product yield is only an 11.5% reduction after four runs. Full article
(This article belongs to the Special Issue Multifunctional Heterogeneous Catalysis)
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15 pages, 1599 KiB  
Article
Stable Continuous Production of γ-Valerolactone from Biomass-Derived Levulinic Acid over Zr–Al-Beta Zeolite Catalyst
by Clara López-Aguado, Marta Paniagua, Juan A. Melero, Jose Iglesias, Pablo Juárez, Manuel López Granados and Gabriel Morales
Catalysts 2020, 10(6), 678; https://doi.org/10.3390/catal10060678 - 17 Jun 2020
Cited by 26 | Viewed by 3860
Abstract
The one-pot conversion of biomass-derived platform molecules such as levulinic acid (LA) and furfural (FAL) into γ-valerolactone (GVL) is challenging because of the need for adequate multi-functional catalysts and high-pressure gaseous hydrogen. As a more sustainable alternative, here we describe the transfer hydrogenation [...] Read more.
The one-pot conversion of biomass-derived platform molecules such as levulinic acid (LA) and furfural (FAL) into γ-valerolactone (GVL) is challenging because of the need for adequate multi-functional catalysts and high-pressure gaseous hydrogen. As a more sustainable alternative, here we describe the transfer hydrogenation of LA to GVL using isopropanol as a hydrogen donor over a Zr-modified beta zeolite catalyst in a continuous fixed-bed reactor. A stable sustained production of GVL was achieved from the levulinic acid, with both high LA conversion (ca. 95%) and GVL yield (ca. 90%), for over at least 20 days in continuous operation at 170 °C. Importantly, the small decay in activity can be advantageously overcome by the means of a simple in situ thermal regeneration in the air atmosphere, leading to a complete recovery of the catalyst activity. Key to this outstanding result is the use of a Zr-modified dealuminated beta zeolite with a tailored Lewis/Brønsted acid sites ratio, which can synergistically catalyze the tandem steps of hydrogen transfer and acid-catalyzed transformations, leading to such a successful and stable production of GVL from LA. Full article
(This article belongs to the Special Issue Multifunctional Heterogeneous Catalysis)
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11 pages, 3130 KiB  
Article
Bifunctional Heterometallic Metal-Organic Frameworks for Solvent-Free Heterogeneous Cascade Catalysis
by Mingming Zheng, Yanxiang Wang and Pingyun Feng
Catalysts 2020, 10(3), 309; https://doi.org/10.3390/catal10030309 - 08 Mar 2020
Cited by 10 | Viewed by 3192
Abstract
A family of heterometallic metal-organic frameworks (MOFs) (CPM200s) harmoniously coexisting as Lewis acids and base (azo) sites were prepared. Seven CPM200s were employed as multifunctional heterogeneous cascade catalysts for the one-pot deacetalization-Knoevenagel reaction in a solvent-free system. Benefiting from the cooperation between Lewis [...] Read more.
A family of heterometallic metal-organic frameworks (MOFs) (CPM200s) harmoniously coexisting as Lewis acids and base (azo) sites were prepared. Seven CPM200s were employed as multifunctional heterogeneous cascade catalysts for the one-pot deacetalization-Knoevenagel reaction in a solvent-free system. Benefiting from the cooperation between Lewis acids from the open metal sites and base sites from the ligands, the CPM200s showed high activity and selectivity for the tandem reaction. The heterometallic 3D porous framework reported here not only offers a combination of two opposite active sites in the same framework of materials but also increases mass transfer of the substrate, thus maximizing the efficiency and substrate selectivity of the bifunctional catalysts. The CPM200s showed the highest turnover frequency (TOF), outperforming that of the reported MOFs in tandem with the deacetalization-Knoevenagel reaction. A strong correlation between the TOF and charge-to-radius ratio (z/r) of metal ions in the CPM200s was observed for the first time. The bifunctional CPM200s catalysts can be reused five times without significant loss of activity. Full article
(This article belongs to the Special Issue Multifunctional Heterogeneous Catalysis)
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19 pages, 7850 KiB  
Article
Facile Mechanochemical Synthesis of Nickel/Graphene Oxide Nanocomposites with Unique and Tunable Morphology: Applications in Heterogeneous Catalysis and Supercapacitors
by Mayakrishnan Gopiraman, Somasundaram Saravanamoorthy, Dian Deng, Andivelu Ilangovan, Ick Soo Kim and Ill Min Chung
Catalysts 2019, 9(5), 486; https://doi.org/10.3390/catal9050486 - 27 May 2019
Cited by 27 | Viewed by 4579
Abstract
In this study, a very simple and highly effective mechanochemical preparation method was developed for the preparation of Ni nanoparticles supported graphene oxide (GO) nanocomposites (Ni/GO, where Ni is a composition of Ni(OH)2, NiOOH, NiO, Ni2O3 and NiO [...] Read more.
In this study, a very simple and highly effective mechanochemical preparation method was developed for the preparation of Ni nanoparticles supported graphene oxide (GO) nanocomposites (Ni/GO, where Ni is a composition of Ni(OH)2, NiOOH, NiO, Ni2O3 and NiO2), 3 wt% NiO/GO (Ni/GO-1) and 8 wt% NiO/GO(Ni/GO-2). The developed method is not only very simple and efficient, but also, the morphology of Ni/GO nanocomposites can be tuned by simply varying the metal loading. Morphology and specific surface area of the resultant Ni/GO nanocomposites were investigated by mean of AFM, HR-TEM and BET. Chemical sate and factual content of Ni in Ni/GO-1 and Ni/GO-2, and the presence of defective sites in Ni-nanocomposites were investigated in detail. To our delight, the prepared Ni/GO-2 demonstrated superior catalytic activity toward the reduction of 2- and 4-nitrophenol in water with high rate constant (kapp) of 35.4 × 10−3 s−1. To the best of our knowledge, this is the best efficient Ni-based graphene nanocomposites for the reduction of 2- and 4-NP reported to date. The Ni/GO-1 and Ni/GO-2 demonstrated an excellent reusability; no loss in its catalytic activity was noticed, even after 10th cycle. Surprisingly the Ni/GO-2 as electrode material exhibited an excellent specific capacitance of 461 F/g in 6 M KOH at a scan rate of 5 mV. Moreover, the Ni/GO nanocomposites were found to possess poor electrical resistance and high stability (no significant change in the specific capacitance even after 1000 cycles). Full article
(This article belongs to the Special Issue Multifunctional Heterogeneous Catalysis)
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