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Heterogeneous Catalysis in Green Chemistry
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Heterogeneous Catalysis in Green Chemistry

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

Deadline for manuscript submissions: closed (10 March 2022) | Viewed by 53556

Special Issue Editors

Dr. Jesús M. Requies

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Guest Editor
Chemical and Environmental Engineering Department, Engineering Faculty of Bilbao, University of Basque Country (UPV/EHU), Plaza Ingeniero Torres Quevedo 1, 48013 Bilbao, Spain
Interests: heterogeneous catalysis; catalyst characterization; biomass; biorefinery; hydrogen; hydrogenolysis; green chemistry
Special Issues, Collections and Topics in MDPI journals
Prof. Dr. José Francisco Cambra Ibáñez

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Guest Editor
Chemical and Environmental Engineering Department. Engineering Faculty of Bilbao, University of Basque Country (UPV/EHU), Plaza Ingeniero Torres Quevedo 1, 48013 Bilbao, Spain
Interests: Heterogeneous catalysis, Hydrotreating, Hydrogen production, Advanced reactor design, CO2 valorisation, clean fuel, biomass to liquids, biomass to gas Name: Dr. Victoria Laura Barrio Cagigal
Dr. Victoria Laura Barrio Cagigal

E-Mail Website
Guest Editor
Chemical and Environmental Engineering Department, Engineering Faculty of Bilbao, University of Basque Country (UPV/EHU), Plaza Ingeniero Torres Quevedo 1, 48013 Bilbao, Spain
Interests: thermocatalytic processes; clean fuels; CO2 valorisation; microreactors and membrane systems; life cycle analysis
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Sustainable development in the chemical industry is based on the recent interest to develop new processes that reduce energy consumption and minimize its environmental impact. Heterogeneous catalysts are the key tool towards Green Chemistry for the production of biofuels and chemicals, reducing the energy consumption and minimizing hazardous products by increasing the activity and selectivity of catalyst to produce chemicals from fossil or renewable raw materials. The development of new and more active and stable catalysts is essential for the implementation of the green chemistry.

This Special Issue will focus on the technological aspects of application of heterogeneous catalysis to the sustainable development. The new developments in the design of heterogeneous catalysts for sustainable processes augur a new knowledge in “Heterogeneous Catalysis in Green Chemistry” that we hope to collect in this Special Issue.

Dr. Jesús M. Requies
Prof. Dr. José Francisco Cambra Ibáñez
Dr. Victoria Laura Barrio Cagigal
Guest Editors

Manuscript Submission Information

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Keywords

  • Heterogeneous catalysts
  • Green chemistry
  • Metal catalysts
  • Biorefinery
  • Biofuels
  • Acid catalysts
  • Functional catalysts
  • Hydrogen technologies
  • Oxidation
  • Hydrotreating
  • Dehydration and hydrogenolysis

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Related Special Issue

Published Papers (11 papers)

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Research

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26 pages, 4028 KiB  
Article
Effect of the Addition of Alkaline Earth and Lanthanide Metals for the Modification of the Alumina Support in Ni and Ru Catalysts in CO2 Methanation
by David Méndez-Mateos, V. Laura Barrio, Jesús M. Requies and José F. Cambra
Catalysts 2021, 11(3), 353; https://doi.org/10.3390/catal11030353 - 9 Mar 2021
Cited by 20 | Viewed by 3584
Abstract
In order to reduce greenhouse gas emissions, which are reaching alarming levels in the atmosphere, capture, recovery, and transformation of carbon dioxide emitted to methane is considered a potentially profitable process. This transformation, known as methanation, is a catalytic reaction that mainly uses [...] Read more.
In order to reduce greenhouse gas emissions, which are reaching alarming levels in the atmosphere, capture, recovery, and transformation of carbon dioxide emitted to methane is considered a potentially profitable process. This transformation, known as methanation, is a catalytic reaction that mainly uses catalysts based on noble metals such as Ru and, although with less efficiency, on transition metals such as Ni. In order to improve the efficiency of these conventional catalysts, the effect of adding alkaline earth metals (Ba, Ca, or Mg at 10 wt%) and lanthanides (La or Ce at 14 wt%) to nickel (13 wt%), ruthenium (1 wt%), or both-based catalysts has been studied at temperatures between 498 and 773 K and 10 bar pressure. The deactivation resistance in presence of H2S was also monitored. The incorporation of La into the catalyst produces interactions between active metal Ni, Ru, or Ru-Ni and the alumina support, as determined by the characterization. This fact results in an improvement in the catalytic activity of the 13Ni/Al2O3 catalyst, which achieves a methane yield of 82% at 680 K for 13Ni/14La-Al2O3, in addition to an increase in H2S deactivation resistance. Furthermore, 89% was achieved for 1Ru-13Ni/14La-Al2O3 at 651 K, but it showed to be more vulnerable to H2S presence. Full article
(This article belongs to the Special Issue Heterogeneous Catalysis in Green Chemistry)
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14 pages, 3780 KiB  
Article
New Approach to Synthesis of Tetralin via Naphthalene Hydrogenation in Supercritical Conditions Using Polymer-Stabilized Pt Nanoparticles
by Alexey V. Bykov, Daria V. Alekseeva, Galina N. Demidenko, Alexandre L. Vasiliev, Linda Nikoshvili and Lioubov Kiwi-Minsker
Catalysts 2020, 10(11), 1362; https://doi.org/10.3390/catal10111362 - 23 Nov 2020
Cited by 19 | Viewed by 3788
Abstract
Supercritical (SC) fluid technologies are well-established methods in modern green chemical synthesis. Using SC fluids as solvents instead of traditional liquids gives benefits of higher diffusivity and lower viscosity, which allows mass transfer intensification and, thus, an increased production rate of chemical transformations. [...] Read more.
Supercritical (SC) fluid technologies are well-established methods in modern green chemical synthesis. Using SC fluids as solvents instead of traditional liquids gives benefits of higher diffusivity and lower viscosity, which allows mass transfer intensification and, thus, an increased production rate of chemical transformations. Therefore, a conjugation of heterogeneous catalysis with SC media is a large step toward a green chemistry. Tetralin (TL) is an important hydrogen donor solvent used for biomass liquefaction. In industry, TL is obtained via catalytic hydrogenation of naphthalene (NL). Herein, for the first time we have demonstrated the NL hydrogenation with close to 100% selectivity to TL at almost full conversion in the SC hexane. The observed transformation rates in SC hexane were much higher allowing process intensification. The downstream processes can be also facilitated since hexane after depressurisation can be easily separated from the reaction products via simple rectification. The TL synthesis was studied in a batch reactor at variation of reaction temperature and overall pressure. For the first time for this process, low Pt-loaded (1 wt.%) nanoparticles stabilized within hyper-cross-linked aromatic polymer (HAP) were applied. The Pt/HAP catalyst was stable under reaction conditions (250 °C, 6 MPa) allowing its recovery and reuse. Full article
(This article belongs to the Special Issue Heterogeneous Catalysis in Green Chemistry)
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14 pages, 862 KiB  
Article
Use of a Reforming Catalyst for Hydrogen Production in the Carbonization Process of Torrefied Biomass
by Alexander Lopez-Urionabarrenechea, Esther Acha, Aitziber Adrados, Jon Solar, Blanca María Caballero and Isabel de Marco
Catalysts 2020, 10(11), 1300; https://doi.org/10.3390/catal10111300 - 10 Nov 2020
Cited by 3 | Viewed by 2638
Abstract
The utilization of charcoal from woody biomass is an efficient way to reduce CO2 emissions from the metallurgical industry. The main aim of this work is to study the charcoal production process from torrefied biomass. For this purpose, torrefaction (3 °C min [...] Read more.
The utilization of charcoal from woody biomass is an efficient way to reduce CO2 emissions from the metallurgical industry. The main aim of this work is to study the charcoal production process from torrefied biomass. For this purpose, torrefaction (3 °C min−1, 250 °C, 30 min) and carbonization (3 °C min−1, 750 °C, 30 min) experiments of eucalyptus wood were carried out in a 3.5 L tank reactor. In the carbonization experiments, a thermo-catalytic treatment of the vaporized phase was also performed, with the objective of producing less condensates and H2-rich gases. The results show that the torrefaction pre-treatment does not affect the chemical properties of charcoal but significantly improves the performance of the carbonization process, where more than 50 wt% of charcoal is obtained. In addition, the thermal and thermo-catalytic treatment of the vaporized phase during the carbonization of torrefied biomass yields better results than in the case of fresh biomass. When torrefied biomass is used as raw material and the reforming catalyst is employed to treat the vapors and gases, a proportion of 71 vol% of H2 in the gases is achieved, together with very low quantities of condensates (8.0 wt%). This allows designing a carbonization process in which, in addition to charcoal, pure H2 can also be produced. Full article
(This article belongs to the Special Issue Heterogeneous Catalysis in Green Chemistry)
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10 pages, 2677 KiB  
Communication
On the Exceptionally High Loading of L-Proline on Multi-Wall Carbon Nanotubes
by Jiafang Xu, Jichao Liang, Sheng Huang, Ge Yang, Keyi Tian, Ruonan Chen, Hongyu Chen and Yanhua Zhang
Catalysts 2020, 10(11), 1246; https://doi.org/10.3390/catal10111246 - 28 Oct 2020
Cited by 2 | Viewed by 2639
Abstract
L-proline is directly loaded on the multi-wall carbon nanotubes (MWCNTs) with exceptionally high loading content of 67 wt.%. The obtained L-proline/MWCNTs catalyst is on par with the catalytic activity of free L-proline, even after 7 rounds of recycling and reusing. The excellent activity [...] Read more.
L-proline is directly loaded on the multi-wall carbon nanotubes (MWCNTs) with exceptionally high loading content of 67 wt.%. The obtained L-proline/MWCNTs catalyst is on par with the catalytic activity of free L-proline, even after 7 rounds of recycling and reusing. The excellent activity of L-proline/MWCNTs in typical Aldol reaction, Mannich reaction, Michael reaction, α-oxyamination reaction, and Knoevenagel condensation shows a broad applicability of the composite catalyst in different reactions and solvent systems. We believe that the unusual loading mode may open a window for designing heterogenized organo-catalysts. Full article
(This article belongs to the Special Issue Heterogeneous Catalysis in Green Chemistry)
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19 pages, 9473 KiB  
Article
An Escape from Noble Metals for Generating Urethanes via Reductive Carbonylation of Nitroarenes over FeSe2/γ-Al2O3 †
by Anh Vy Tran, Thuy Tram Huynh Nguyen, Thanh Tung Nguyen, Hye Jin Lee, Jayeon Baek and Yong Jin Kim
Catalysts 2020, 10(11), 1228; https://doi.org/10.3390/catal10111228 - 22 Oct 2020
Cited by 4 | Viewed by 3185
Abstract
The reaction of FeCl3, SeO2, and Pyridine (Py) in the presence of methanol (MeOH) under CO pressure generates a black precipitate, which has been confirmed as ferric di-selenide, FeSe2 through different structure characterization methods. Furthermore, impregnation of 5 [...] Read more.
The reaction of FeCl3, SeO2, and Pyridine (Py) in the presence of methanol (MeOH) under CO pressure generates a black precipitate, which has been confirmed as ferric di-selenide, FeSe2 through different structure characterization methods. Furthermore, impregnation of 5 wt% of FeSe2 onto γ-Al2O3 exhibits better catalytic performance than FeSe2 due to the highly dispersed and smaller particle sizes ca. 200–300 nm. The reductive carbonylation of nitrobenzene (NB) was investigated over FeSe2/γ-Al2O3 as a heterogeneous catalyst, delivering an excellent yield and high selectivity of methyl-N-phenyl carbamate (MPC). Moreover, a set of reactions was performed with variation in the reaction time, temperature, and pressure to investigate the effects of these factors. In particular, FeSe2/γ-Al2O3 is highly stable and can be recycled for up to five cycles without significant loss in catalytic performance. A mechanistic study was also conducted on this low-cost catalyst system, especially proposing a crucial role of FeSe2 (μ-CO) active species. Full article
(This article belongs to the Special Issue Heterogeneous Catalysis in Green Chemistry)
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18 pages, 4398 KiB  
Article
Ammonium Salts Catalyzed Acetalization Reactions in Green Ethereal Solvents
by Ugo Azzena, Massimo Carraro, Martina Corrias, Rosella Crisafulli, Lidia De Luca, Silvia Gaspa, Luca Nuvoli, Salvatore Pintus, Luisa Pisano, Riccardo Polese, Michela Sanna, Giuseppe Satta, Nina Senes, Luigi Urtis and Sebastiano Garroni
Catalysts 2020, 10(10), 1108; https://doi.org/10.3390/catal10101108 - 24 Sep 2020
Cited by 5 | Viewed by 3308
Abstract
Cyclopentyl methyl ether and 2-methyltetrahydrofuran, low impact ethereal solvents forming a positive azeotrope with water, were successfully employed as solvents in the synthesis of a variety of acetals carried out under Dean–Stark conditions in the presence of heterogeneous acidic catalysts. Under these conditions, [...] Read more.
Cyclopentyl methyl ether and 2-methyltetrahydrofuran, low impact ethereal solvents forming a positive azeotrope with water, were successfully employed as solvents in the synthesis of a variety of acetals carried out under Dean–Stark conditions in the presence of heterogeneous acidic catalysts. Under these conditions, ammonium salts, either as such or supported on SiO2, performed better or equally well than widely employed homogeneous and heterogeneous acidic catalysts such as p-toluenesulfonic acid, Amberlyst 15®, or Montmorillonite K10. Several examples highlight the advantage of tuning the relative acidities of ammonium salts by appropriately selecting the counterion. Within one of these examples, our protocol clearly outweighs the classic p-toluenesulfonic acid/toluene protocol in terms of chemoselectivity. Silica-supported catalysts were characterized by SEM, TEM, and FTIR spectroscopies, as well as by N2 physisorption. Such a characterization reveals an even distribution of ammonium salts on silica, thus confirming the formation of expected catalytic supports. Full article
(This article belongs to the Special Issue Heterogeneous Catalysis in Green Chemistry)
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13 pages, 4979 KiB  
Article
Study the Effect of Various Sulfonation Methods on Catalytic Activity of Carbohydrate-Derived Catalysts for Ester Production
by Nur Hidayah Deris, Umer Rashid, Soroush Soltani, Thomas Shean Yaw Choong and Imededdine Arbi Nehdi
Catalysts 2020, 10(6), 638; https://doi.org/10.3390/catal10060638 - 8 Jun 2020
Cited by 9 | Viewed by 3922
Abstract
In the present study, four types of sulfonation method, including thermal treatment with concentrated sulfuric acid (H2SO4), thermal decomposition of ammonium sulphate (NHSO4), thermal treatment with chlorosulfonic in chloroform (HSO3Cl), and in situ polymerization [...] Read more.
In the present study, four types of sulfonation method, including thermal treatment with concentrated sulfuric acid (H2SO4), thermal decomposition of ammonium sulphate (NHSO4), thermal treatment with chlorosulfonic in chloroform (HSO3Cl), and in situ polymerization of poly(sodium4-styrenesulfonate) (PSS), were employed to convert incomplete carbonized glucose (ICG) to sulfonated heterogeneous catalysts for the fatty acid methyl ester (FAME) production. The characteristics of synthesized catalysts were further examined using Raman spectroscopy, Fourier transformation infrared (FT-IR), ammonia temperature programmed desorption (NH3-TPD), Brunauer–Emmett–Teller (BET), thermogravimetric analysis (TGA), scanning electron microscopy (SEM), and energy dispersive X-ray (EDX). According to experiments, the sulfonic acid density was varied in a range from 4.408 to 14.643 mmol g−1 over various sulfonation methods. The catalytic activity of synthesized catalysts over different sulfonation methods was determined by performing the conversion of palm fatty acid distillate (PFAD) to ester synthesis in a batch-system reactor. The findings reveal that using PSS-ICG resulted in the highest FAME yield of 96.3% followed by HSO3Cl-ICG of 94.8%, NHSO4-ICG of 84.2%; and H2SO4-ICG of 77.2%. According to results, the ICG sulfonated by PSS method with the highest acid density (14.643 mmol g−1) gave the highest catalytic activity over PFAD conversion to biodiesel. According to experiment results, acid density played a crucial role over FAME yield percentage. Besides acid density, it is also worth mentioning that various sulfonation methods including different mechanisms, chemicals and sulfonating agents played crucial roles in the FAME yield percentage. Full article
(This article belongs to the Special Issue Heterogeneous Catalysis in Green Chemistry)
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Review

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34 pages, 2860 KiB  
Review
Recent Advances in Catalysis for Methanation of CO2 from Biogas
by Selina Nieß, Udo Armbruster, Sebastian Dietrich and Marco Klemm
Catalysts 2022, 12(4), 374; https://doi.org/10.3390/catal12040374 - 25 Mar 2022
Cited by 22 | Viewed by 5590
Abstract
Biogas, with its high carbon dioxide content (30–50 vol%), is an attractive feed for catalytic methanation with green hydrogen, and is suitable for establishing a closed carbon cycle with methane as energy carrier. The most important questions for direct biogas methanation are how [...] Read more.
Biogas, with its high carbon dioxide content (30–50 vol%), is an attractive feed for catalytic methanation with green hydrogen, and is suitable for establishing a closed carbon cycle with methane as energy carrier. The most important questions for direct biogas methanation are how the high methane content influences the methanation reaction and overall efficiency on one hand, and to what extent the methanation catalysts can be made more resistant to various sulfur-containing compounds in biogas on the other hand. Ni-based catalysts are the most favored for economic reasons. The interplay of active compounds, supports, and promoters is discussed regarding the potential for improving sulfur resistance. Several strategies are addressed and experimental studies are evaluated, to identify catalysts which might be suitable for these challenges. As several catalyst functionalities must be combined, materials with two active metals and binary oxide support seem to be the best approach to technically applicable solutions. The high methane content in biogas appears to have a measurable impact on equilibrium and therefore CO2 conversion. Depending on the initial CH4/CO2 ratio, this might lead to a product with higher methane content, and, after work-up, to a drop in-option for existing natural gas grids. Full article
(This article belongs to the Special Issue Heterogeneous Catalysis in Green Chemistry)
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9 pages, 1165 KiB  
Review
Solid Acid Catalysts for the Hock Cleavage of Hydroperoxides
by Jan Drönner, Peter Hausoul, Regina Palkovits and Matthias Eisenacher
Catalysts 2022, 12(1), 91; https://doi.org/10.3390/catal12010091 - 14 Jan 2022
Cited by 11 | Viewed by 5758
Abstract
The oxidation of cumene and following cleavage of cumene hydroperoxide (CHP) with sulfuric acid (Hock rearrangement) is still, by far, the dominant synthetic route to produce phenol. In 2020, the global phenol market reached a value of 23.3 billion US$ with a projected [...] Read more.
The oxidation of cumene and following cleavage of cumene hydroperoxide (CHP) with sulfuric acid (Hock rearrangement) is still, by far, the dominant synthetic route to produce phenol. In 2020, the global phenol market reached a value of 23.3 billion US$ with a projected compound annual growth rate of 3.4% for 2020–2025. From ecological and economical viewpoints, the key step of this process is the cleavage of CHP. One sought-after way to likewise reduce energy consumption and waste production of the process is to substitute sulfuric acid with heterogeneous catalysts. Different types of zeolites, silicon-based clays, heteropoly acids, and ion exchange resins have been investigated and tested in various studies. For every type of these solid acid catalysts, several materials were found that show high yield and selectivity to phenol. In this mini-review, first a brief introduction and overview on the Hock process is given. Next, the mechanism, kinetics, and safety aspects are summarized and discussed. Following, the different types of heterogeneous catalysts and their performance as catalyst in the Hock process are illustrated. Finally, the different approaches to substitute sulfuric acid in the synthetic route to produce phenol are briefly concluded and a short outlook is given. Full article
(This article belongs to the Special Issue Heterogeneous Catalysis in Green Chemistry)
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15 pages, 1792 KiB  
Review
Waste Animal Bones as Catalysts for Biodiesel Production; A Mini Review
by Fayaz Hussain, Saad Alshahrani, Muhammad Mujtaba Abbas, Haris Mahmood Khan, Asif Jamil, Haseeb Yaqoob, Manzoore Elahi M. Soudagar, Muhammad Imran, Mushtaq Ahmad and Mamoona Munir
Catalysts 2021, 11(5), 630; https://doi.org/10.3390/catal11050630 - 13 May 2021
Cited by 51 | Viewed by 10421
Abstract
Slaughterhouse waste is considered to be an emerging issue because of its disposal cost. As an alternative, it would be a great prospect for the bioeconomy society to explore new usages of these leftover materials. As per food safety rules mentioned by EU [...] Read more.
Slaughterhouse waste is considered to be an emerging issue because of its disposal cost. As an alternative, it would be a great prospect for the bioeconomy society to explore new usages of these leftover materials. As per food safety rules mentioned by EU legislation, all bone waste generated by slaughterhouses ought to be disposed of by rendering. The huge quantity of worldwide bone waste generation (130 billion kilograms per annum) is an environmental burden if not properly managed. The waste animal bones can be efficiently employed as a heterogeneous catalyst to produce biodiesel. This mini review summarized the recent literature reported for biodiesel generation using waste animal bones derived heterogeneous catalyst. It discusses the sources of bone waste, catalyst preparation methods, particularly calcination and its effects, and important characteristics of bones derived catalyst. It suggests that catalysts extracted from waste animal bones have suitable catalytic activity in transesterification of different oil sources to generate a good quality biodiesel. Full article
(This article belongs to the Special Issue Heterogeneous Catalysis in Green Chemistry)
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25 pages, 2166 KiB  
Review
Value-Added Bio-Chemicals Commodities from Catalytic Conversion of Biomass Derived Furan-Compounds
by Aitziber Iriondo, Ion Agirre, Nerea Viar and Jesús Requies
Catalysts 2020, 10(8), 895; https://doi.org/10.3390/catal10080895 - 7 Aug 2020
Cited by 23 | Viewed by 5454
Abstract
The depletion of fossil resources in the near future and the need to decrease greenhouse gas emissions lead to the investigation of using alternative renewable resources as raw materials. One of the most promising options is the conversion of lignocellulosic biomass (like forestry [...] Read more.
The depletion of fossil resources in the near future and the need to decrease greenhouse gas emissions lead to the investigation of using alternative renewable resources as raw materials. One of the most promising options is the conversion of lignocellulosic biomass (like forestry residues) into bioenergy, biofuels and biochemicals. Among these products, the production of intermediate biochemicals has become an important goal since the petrochemical industry needs to find sustainable alternatives. In this way, the chemical industry competitiveness could be improved as bioproducts have a great potential market. Thus, the main objective of this review is to describe the production processes under study (reaction conditions, type of catalysts, solvents, etc.) of some promising intermediate biochemicals, such as; alcohols (1,2,6-hexanetriol, 1,6-hexanetriol and pentanediols (1,2 and 1,5-pentanediol)), maleic anhydride and 5-alkoxymethylfuran. These compounds can be produced using 5-hydroxymethylfurfural and/or furfural, which they both are considered one of the main biomass derived building blocks. Full article
(This article belongs to the Special Issue Heterogeneous Catalysis in Green Chemistry)
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