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Special Issue "Catalysis: Providing Sustainable Solutions to Global Challenges"

A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Green Chemistry".

Deadline for manuscript submissions: 15 April 2019

Special Issue Editors

Guest Editor
Prof. Dr. Robert Raja

School of Chemistry, Faculty of Natural and Environmental Sciences, University of Southampton, University Road, Southampton SO17 1BJ, UK
Website | E-Mail
Interests: heterogeneous catalysis; hybrid materials; renewable energy; CO2 utilization; sustainable chemistry; multifunctional asymmetric catalysis; synergistic nanoparticles; solid-acid catalysis
Assistant Guest Editor
Dr. Matthew E. Potter

School of Chemistry, Faculty of Natural and Environmental Sciences, University of Southampton, University Road, Southampton SO17 1BJ, UK
Website | E-Mail
Interests: heterogeneous catalysis; CO2 utilization; CO2 capture; nanoparticle design; synchrotron-based characterization; in situ characterization; solid-acid catalysis
Assistant Guest Editor
Ms. Stephanie Chapman

School of Chemistry, Faculty of Natural and Environmental Sciences, University of Southampton, University Road, Southampton SO17 1BJ, UK
E-Mail
Interests: heterogeneous catalysis; solid-acid catalysts; zeotype framework materials; multifunctional hierarchically-porous architectures; advanced characterization; synchrotron-based spectroscopy; sustainable transformations

Special Issue Information

Dear Colleagues,

The growing demands of society are placing an intense strain on our energy resources and environmental sustainability. Cutting-edge research, allied with sustainable industrial practices, can provide a platform for confronting global challenges, thereby affording equitable research solutions for future generations. In addressing some of the major issues relating to climate change, healthcare, nutrition and energy, catalysis has outgrown its traditional boundaries. Beyond simply accelerating chemical processes, recent advances in molecular scale design and operando spectroscopy have seen developments in progressive fields such as photo- and electro-catalysis. The discovery of hybrid catalytic materials has provided stimulus for expanding the horizons of Green Chemistry and Sustainable Technology, conferring a greater impetus in the utilization of renewable feedstocks and in bifunctional and cooperative catalysis. In parallel, advances in atomic scale characterization are offering new mechanistic insights at the molecular level, facilitating the intelligent design of targeted catalysts for the chemical industry. In all, catalysis has earned its place at the forefront of Green Chemistry, harnessing advances in renewable energy generation, biomass transformation, and CO2 storage and utilization, for creating a sustainable world.

This Special Issue of Molecules has been commissioned as a platform for scientists to highlight their advances in the field of Sustainable Catalysis. This unique collection of research articles aims to portfolio innovative, pioneering developments in molecular scale catalyst design and characterization, which will provide a comprehensive overview of advances in the field, affording exclusive insights on sustainability for academics and research students. We therefore invite you to submit a full paper, short communication, or review article to support this Special Issue, "Catalysis: Providing Sustainable Solutions to Global Challenges".

Prof. Dr. Robert Raja
Guest Editor

Dr. Matthew E. Potter
Ms. Stephanie Chapman
Assistant 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 papers will be 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. Molecules is an international peer-reviewed open access semimonthly 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 1800 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

  • Sustainable Catalytic Solutions
  • Green Chemistry
  • Heterogeneous Catalysis
  • Environmental Sustainability
  • Sustainable Chemicals and Polymers
  • Biomass Transformation and Valorisation
  • Alternative Energy
  • Photocatalysis
  • Renewable Energy
  • Molecular Design
  • CO2 Utilisation and Storage
  • Operando Spectroscopy
  • Ionic Liquids in Catalysis
  • Electrocatalysis
  • Renewable Feedstocks
  • Hybrid Materials and Processes
  • Global Challenges and Sustainability
  • Bifunctional and Cooperative Catalysis
  • Molecular scale characterisation

Published Papers (7 papers)

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Research

Jump to: Review

Open AccessFeature PaperArticle Influence of Silicodactyly in the Preparation of Hybrid Materials
Molecules 2019, 24(5), 848; https://doi.org/10.3390/molecules24050848
Received: 30 January 2019 / Revised: 15 February 2019 / Accepted: 26 February 2019 / Published: 28 February 2019
PDF Full-text (4373 KB) | HTML Full-text | XML Full-text | Supplementary Files
Abstract
The organic–inorganic hybrid materials have attracted great attention due to their improved or unusual properties that open promising applications in different areas such as optics, electronics, energy, environment, biology, medicine and heterogeneous catalysis. Different types of silicodactyl platforms grafted on silica inorganic supports [...] Read more.
The organic–inorganic hybrid materials have attracted great attention due to their improved or unusual properties that open promising applications in different areas such as optics, electronics, energy, environment, biology, medicine and heterogeneous catalysis. Different types of silicodactyl platforms grafted on silica inorganic supports can be used to synthesize hybrid materials. A careful evaluation of the dactyly of the organic precursors, normally alkoxysilanes, and of the type of interaction with the inorganic supports is presented. In fact, depending on the hydrophilicity of the silica surface (e.g., number and density of surface silanols) as well as on the grafting conditions, the hydrolysis and condensation reaction of the silylated moieties can involve only one or two out of three alkoxysilane groups. The influence of silicodactyly in the preparation of organic-inorganic silica-based hybrids is studied by TGA, 29Si, 1H and 13C solid-state NMR and FTIR spectroscopies, with the support of Molecular Dynamics calculations. Computational studies are used to forecast the influence of the different grafting configurations on the tendency of the silane to stick on the inorganic surface. Full article
(This article belongs to the Special Issue Catalysis: Providing Sustainable Solutions to Global Challenges)
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Open AccessArticle Morphology-Dependent Catalytic Activity of Ru/CeO2 in Dry Reforming of Methane
Molecules 2019, 24(3), 526; https://doi.org/10.3390/molecules24030526
Received: 31 December 2018 / Revised: 24 January 2019 / Accepted: 29 January 2019 / Published: 1 February 2019
PDF Full-text (4605 KB) | HTML Full-text | XML Full-text | Supplementary Files
Abstract
Three morphology-controlled CeO2, namely nanorods (NRs), nanocubes (NCs), and nanopolyhedra (NPs), with different mainly exposed crystal facets of (110), (100), and (111), respectively, have been used as supports to prepare Ru (3 wt.%) nanoparticle-loaded catalysts. The catalysts were characterized by H [...] Read more.
Three morphology-controlled CeO2, namely nanorods (NRs), nanocubes (NCs), and nanopolyhedra (NPs), with different mainly exposed crystal facets of (110), (100), and (111), respectively, have been used as supports to prepare Ru (3 wt.%) nanoparticle-loaded catalysts. The catalysts were characterized by H2-temperature programmed reduction (H2-TPR), CO– temperature programmed desorption (CO-TPD), N2 adsorption–desorption, X-ray diffraction (XRD), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), and high-resolution transmission electron microscopy (HRTEM) and energy-dispersive X-ray spectroscopy (XDS). The characterization results showed that CeO2-NRs, CeO2-NCs, and CeO2-NPs mainly expose (110), (100) and (111) facets, respectively. Moreover, CeO2-NRs and CeO2-NCs present higher oxygen vacancy concentration than CeO2-NPs. In the CO2 reforming of methane reaction, Ru/CeO2-NR and Ru/CeO2-NC catalysts showed better catalytic performance than Ru/CeO2-NPs, indicating that the catalysts with high oxygen vacancy concentration are beneficial for promoting catalytic activity. Full article
(This article belongs to the Special Issue Catalysis: Providing Sustainable Solutions to Global Challenges)
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Open AccessFeature PaperArticle CNF-Functionalization as Versatile Tool for Tuning Activity in Cellulose-Derived Product Hydrogenation
Molecules 2019, 24(2), 316; https://doi.org/10.3390/molecules24020316
Received: 2 January 2019 / Revised: 11 January 2019 / Accepted: 12 January 2019 / Published: 16 January 2019
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Abstract
Carbon nanofibers (CNFs) have been functionalized by introducing O, N, and P containing groups in order to investigate the effect of support functionalization in Ru catalysed hydroxymethyl furfural (HMF) and levulinic acid (LA) hydrogenation. In the case of HMF, despite the fact that [...] Read more.
Carbon nanofibers (CNFs) have been functionalized by introducing O, N, and P containing groups in order to investigate the effect of support functionalization in Ru catalysed hydroxymethyl furfural (HMF) and levulinic acid (LA) hydrogenation. In the case of HMF, despite the fact that no effect on selectivity was observed (all the catalysts produced selectively gamma-valerolactone (GVL)), the functionalization strongly affected the activity of the reaction. O-containing and N-containing supports presented a higher activity compared to the bare support. On the contrary, in HMF hydrogenation, functionalization of the support did not have a beneficial effect on the activity of a Ru-catalysed reaction with respect to bare support and only CNFs-O behaved similarly to bare CNFs. In fact, when CNFs-N or CNFs-P were used as the supports, a lower activity was observed, as well as a change in selectivity in which the production of ethers (from the reaction with the solvent) greatly increased. Full article
(This article belongs to the Special Issue Catalysis: Providing Sustainable Solutions to Global Challenges)
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Open AccessFeature PaperArticle Laminaria digitata and Palmaria palmata Seaweeds as Natural Source of Catalysts for the Cycloaddition of CO2 to Epoxides
Molecules 2019, 24(2), 269; https://doi.org/10.3390/molecules24020269
Received: 11 December 2018 / Revised: 3 January 2019 / Accepted: 9 January 2019 / Published: 12 January 2019
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Abstract
Seaweed powder has been found to act as an effective catalyst for the fixation of CO2 into epoxides to generate cyclic carbonates under solvent free conditions. Model background reactions were performed using metal halides and amino acids typically found in common seaweeds [...] Read more.
Seaweed powder has been found to act as an effective catalyst for the fixation of CO2 into epoxides to generate cyclic carbonates under solvent free conditions. Model background reactions were performed using metal halides and amino acids typically found in common seaweeds which showed potassium iodide (KI) to be the most active. The efficacy of the seaweed catalysts kelp (Laminaria digitata) and dulse (Palmaria palmata) was probed based on particle size, showing that kelp possessed greater catalytic ability, achieving a maximum conversion and selectivity of 63.7% to styrene carbonate using a kelp loading of 80% by weight with respect to epoxide, 40 bar of CO2, 120 °C for 3 h. Maximizing selectivity was difficult due to the generation of diol side product from residual H2O found in kelp, along with a chlorinated by-product thought to form due to a high quantity of chloride salts in the seaweeds. Data showed there was loss of organic matter upon use of the kelp catalyst, likely due to the breakdown of organic compounds and their subsequent removal during product extraction. This was highlighted as the likely cause of loss of catalytic activity upon reuse of the Kelp catalyst. Full article
(This article belongs to the Special Issue Catalysis: Providing Sustainable Solutions to Global Challenges)
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Review

Jump to: Research

Open AccessFeature PaperReview Functionalized Periodic Mesoporous Organosilicas: Tunable Hydrophobic Solid Acids for Biomass Conversion
Molecules 2019, 24(2), 239; https://doi.org/10.3390/molecules24020239
Received: 29 November 2018 / Revised: 28 December 2018 / Accepted: 4 January 2019 / Published: 10 January 2019
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Abstract
The catalytic deoxygenation of bio-based feedstocks to fuels and chemicals presents new challenges to the catalytic scientist, with many transformations either performed in or liberating water as a byproduct during reaction. The design of catalysts with tunable hydrophobicity to aid product and reactant [...] Read more.
The catalytic deoxygenation of bio-based feedstocks to fuels and chemicals presents new challenges to the catalytic scientist, with many transformations either performed in or liberating water as a byproduct during reaction. The design of catalysts with tunable hydrophobicity to aid product and reactant adsorption or desorption, respectively, is vital for processes including (trans)esterification and condensation reactions employed in sustainable biodiesel production and bio-oil upgrading processes. Increasing surface hydrophobicity of catalyst materials offers a means to displace water from the catalyst active site, and minimizes potential deactivation or hydrolysis side reactions. Hybrid organic–inorganic porous solids offer exciting opportunities to tune surface polarity and hydrophobicity, as well as critical parameters in controlling adsorption, reactant activation, and product selectivity in liquid and vapor phase catalysis. Here, we review advances in the synthesis and application of sulfonic-acid-functionalized periodic mesoporous organosilicas (PMO) as tunable hydrophobic solid acid catalysts in reactions relevant to biorefining and biofuel production. Full article
(This article belongs to the Special Issue Catalysis: Providing Sustainable Solutions to Global Challenges)
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Open AccessReview Catalytic Conversion of Carbon Dioxide through C-N Bond Formation
Molecules 2019, 24(1), 182; https://doi.org/10.3390/molecules24010182
Received: 1 December 2018 / Revised: 19 December 2018 / Accepted: 4 January 2019 / Published: 5 January 2019
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Abstract
From the viewpoint of green chemistry and sustainable development, it is of great significance to synthesize chemicals from CO2 as C1 source through C-N bond formation. During the past several decade years, many studies on C-N bond formation reaction were involved, [...] Read more.
From the viewpoint of green chemistry and sustainable development, it is of great significance to synthesize chemicals from CO2 as C1 source through C-N bond formation. During the past several decade years, many studies on C-N bond formation reaction were involved, and many efforts have been made on the theory. Nevertheless, several great challenges such as thermodynamic limitation, low catalytic efficiency and selectivity, and high pressure etc. are still suffered. Herein, recent advances are highlighted on the development of catalytic methods for chemical fixation of CO2 to various chemicals through C-N bond formation. Meanwhile, the catalytic systems (metal and metal-free catalysis), strategies and catalytic mechanism are summarized and discussed in detail. Besides, this review also covers some novel synthetic strategies to urethanes based on amines and CO2. Finally, the regulatory strategies on functionalization of CO2 for N-methylation/N-formylation of amines with phenylsilane and heterogeneous catalysis N-methylation of amines with CO2 and H2 are emphasized. Full article
(This article belongs to the Special Issue Catalysis: Providing Sustainable Solutions to Global Challenges)
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Open AccessReview Metal Organic Frameworks Based Materials for Heterogeneous Photocatalysis
Molecules 2018, 23(11), 2947; https://doi.org/10.3390/molecules23112947
Received: 15 October 2018 / Revised: 7 November 2018 / Accepted: 9 November 2018 / Published: 12 November 2018
Cited by 1 | PDF Full-text (4880 KB) | HTML Full-text | XML Full-text
Abstract
The increase in environmental pollution due to the excessive use of fossil fuels has prompted the development of alternative and sustainable energy sources. As an abundant and sustainable energy, solar energy represents the most attractive and promising clean energy source for replacing fossil [...] Read more.
The increase in environmental pollution due to the excessive use of fossil fuels has prompted the development of alternative and sustainable energy sources. As an abundant and sustainable energy, solar energy represents the most attractive and promising clean energy source for replacing fossil fuels. Metal organic frameworks (MOFs) are easily constructed and can be tailored towards favorable photocatalytic properties in pollution degradation, organic transformations, CO2 reduction and water splitting. In this review, we first summarize the different roles of MOF materials in the photoredox chemical systems. Then, the typical applications of MOF materials in heterogeneous photocatalysis are discussed in detail. Finally, the challenges and opportunities in this promising field are evaluated. Full article
(This article belongs to the Special Issue Catalysis: Providing Sustainable Solutions to Global Challenges)
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Planned Papers

The below list represents only planned manuscripts. Some of these manuscripts have not been received by the Editorial Office yet. Papers submitted to MDPI journals are subject to peer-review.

Type: Article
Title: Carbon functionalisation as tool for cellulose transformation
Author: Laura Prati
Abstract: The direct cellulose transformation is still representing a big challenge. The paper focuses on the role of different functionalisations introduced on carbon surface in the depolimerisation/dehydration of cellulose. Carbons which differ for surface area, porosity and functionalities have been evaluated under different reaction conditions for testing their activity and selectivity but also resistance to several cycle of uses.

 

Type: Review
Title: Metal Organic Frameworks in Photocatalysis
Author: Shu-Na Zhao 1, 2, Dirk Poelman 2 and Pascal Van Der Voort 1,*
Affiliation:
1   Department of Chemistry, Center for Ordered Materials, Organometallics and Catalysis (COMOC), Ghent University, Krijgslaan 281 (S3), 9000 Gent, Belgium; [email protected]
2   LumiLab, Department of Solid State Sciences, Ghent University, Krijgslaan 281 (S1), 9000 Gent, Belgium; [email protected]
*   Correspondence: [email protected]; Tel.: +32-9-264-44-42
Abstract: The increase in environmental problems has prompted the development of alternative and sustainable energy sources. Sunlight represents a very attractive clean energy source for replacing fossil fuels.
Metal-Organic Frameworks have emerged in the last decade as very promising versatile materials, as they are highly porous, crystalline and easily tunable. They are constructed through inorganic nodes (metal ions, metal oxide clusters, …) that are connected by multitopic, rigid organic linkers (e.g. benzene dicarboxylate). They have been successfully used in gas storage, gas separation, sensing, heterogeneous catalysis, luminescence, etc. Currently big companies alongside many small startups are fully exploring the industrial applications of MOFs.
Herein, we discuss the different roles that MOFs can play in photocatalysis, including pollutant abatement, synthetic photocatalytic reactions, photo-electro-catalytic cells, water splitting and CO2 conversion.

Title: Influence of Silicodactyly in the Preparation of Hybrid Materials
Authors: C. Ivaldi, I. Miletto, G. Paul, G.B. Giovenzana, M. Cossi, L. Marchese, E. Gianotti*
Abstract: The organic–inorganic hybrid materials have attracted great attention due to their improved or unusual properties that open promising applications in different areas such as optics, electronics, energy, environment, biology, medicine and heterogeneous catalysis.
Different types of silicodactyls and multipodal platforms, based on different backbones, grafted on silica inorganic supports will be used to synthesize hybrid materials. A careful evaluation of the dactyly and of the type of interaction with the inorganic supports will be presented. In fact, depending on the hydrophilicity of the silica surface (e.g. number and density of surface silanols) as well as on the grafting conditions, the hydrolysis and condensation reaction of the sylilated moieties can involve only one or two out of three alkoxysilane groups. The influence of silicodactyly in the preparation of organic-inorganic silica based hybrids will be studied by 29Si, 1H and 13C solid-state NMR and FTIR spectroscopy, with the support of ab initio calculations. Computational study will be used to forecast the influence of the different grafting configurations on the tendency of the silane to stick on the silica surface. 

Type: Article
Title: Morphology-dependent catalytic activity of Ru/CeO2 in dry reforming of methane
Author: Heyong He
Abstract: Three morphologically controlled CeO2, namely nanorods (NRs), nanocubes (NCs) and nanopolyhedrons (NPs) CeO2 have been used as supports to prepare nanoparticle Ru (3 wt.%) catalysts. The catalysts were characterized by H2-temperature programmed reduction (H2-TPR), N2 adsorption-desorption, X-ray diffraction (XRD), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM). The characterization results show that CeO2-NRs, CeO2-NCs and CeO2-NPs exposes mainly (110) (100) and (111) facets, respectively, and CeO2-NRs and CeO2-NCs present higher oxygen vacancy concentration than CeO2-NPs. In the CO2 reforming of methane reaction, Ru/CeO2-NRs and Ru/CeO2-NCs catalysts showed better catalytic performance than Ru/CeO2-NPs, indicating that the catalysts with more oxygen vacancies concentration are beneficial to promote the catalytic activity.

Type: Review
Title: Recent advances in catalytic conversion of carbon dioxide through C-N bond formation
Authors: Jing-Yuan Li, Qing-Wen Song, Ping Liu, and Kan Zhang
Abstract: Carbon dioxide, “problematic” toward the activities of human beings, is of importance C1 feedstock due to its cheap, abundant and relatively nontoxic. Although it is an ideal carbon source, its chemical transformations have not been widely developed so far and are still far from synthetic applications, especially in the construction of valuable chemicals. This review summarizes the recent advances (2012-2018) in catalytic conversion of CO2 through C-N bond formation and their synthetic application. This review covers typical catalytic transformation of CO2 via amidation to prepare valuable compounds with the improved atom economy and enhanced sustainability of chemical processes.

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