Special Issue "Mesostructured Materials and Their Catalytic Applications"

A special issue of Catalysts (ISSN 2073-4344).

Deadline for manuscript submissions: closed (30 April 2017)

Special Issue Editors

Guest Editor
Prof. Dr. Adam F. Lee

European Bioenergy Research Institute, Aston University, Aston Triangle, Birmingham B4 7ET, UK
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Interests: surface science; heterogeneous catalysis; green chemistry; synchrotron radiation; porous solids; nanoparticles; alloys; selective oxidation; biofuels
Guest Editor
Dr. Jean-Philippe Dacquin

Catalytic Materials Team (MATCAT), C4 Building, Unité de Catalyse et de Chimie du Solide (UCCS), UMR CNRS 8181, Université Lille 1, Science et Technologies, France
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Guest Editor
Prof. Karen Wilson

European Bioenergy Research Institute, Aston University, Aston Triangle, Birmingham B4 7ET, UK
Website | E-Mail

Special Issue Information

Dear Colleagues,

Rational design of nanostructured materials with tunable physicochemical properties is critical to the successful development of next-generation heterogeneous catalysts with enhanced performance. The introduction of (controlled) porosity into catalysts is one of the most popular approaches to increasing the density of surface active sites available for chemical transformations, exemplified by crystalline microporous materials such as zeolites and metal-organic frameworks. However, growing interest in the use of bulky, bio-derived feedstocks, and desire for intensified and sustainable processes, underpinned by academic and industrial synergies across the chemistry-chemical engineering interface, is driving the synthesis and application of larger mesoporous solid catalysts with superior mass-transport properties to their microporous counterparts. Classes of mesoporous heterogenous catalysts with well-defined and controlled porosity, including inorganic metal oxides, carbons and cross-linked polymers, are of particularly promising interest for liquid phase reactions wherein pore dimensions and connectivity offer size- and or-shape selectivity, in addition to enhanced dispersion of high active sites and/or reactant and product in-pore diffusion.

This Special Issue will feature articles on the synthesis and application of catalysts with controlled mesoporosity (excluding materials whose porosity simply arises through interparticle voids) wherein novelty arises from any of the following: (i) the synthesis of new mesoporous and/or hierarchical mesoporous catalysts; (ii) new methods to incorporate catalytically active functionalities within mesoporous architectures, including acid, base, metal, oxide and organic moieties; (iii) the application of known mesoporous catalysts to new transformations for which their porosity confers enhanced activity, selectivity and/or stability. Mesoporous frameworks including metal oxides, metals, carbons, polymers and associated composites of these are all of interest.

Prof. Dr. Adam F. Lee
Professor Karen Wilson
Dr. Jean-Philippe Dacquin
Guest Editor

Manuscript Submission Information

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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 1000 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

  • Heterogeneous catalysis
  • Porous solid
  • Hierarchical
  • Oxide
  • Polymer
  • Zeolite
  • Green chemistry
  • Carbon
  • Polymer

Published Papers (7 papers)

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Research

Open AccessFeature PaperArticle Mo(VI) Complexes Immobilized on SBA-15 as an Efficient Catalyst for 1-Octene Epoxidation
Catalysts 2017, 7(7), 215; doi:10.3390/catal7070215
Received: 13 June 2017 / Revised: 8 July 2017 / Accepted: 11 July 2017 / Published: 18 July 2017
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Abstract
SBA-15 materials were functionalized through a post-synthetic methodology with molybdenum-Schiff bases to provide catalytic activity in epoxidation reactions. Thus, glycidoxypropyl functionalities were first attached to the surface of the mesostructured silica, followed by the reaction of the immobilized oxirane groups with 2-amino propyl
[...] Read more.
SBA-15 materials were functionalized through a post-synthetic methodology with molybdenum-Schiff bases to provide catalytic activity in epoxidation reactions. Thus, glycidoxypropyl functionalities were first attached to the surface of the mesostructured silica, followed by the reaction of the immobilized oxirane groups with 2-amino propyl pyridine. This reaction allowed the obtaining of (hydroxypropyl)-2-aminomethyl pyridine ligands, directly tethered to the surface of the mesoporous silica-based SBA-15, which resulted in excellent chelating ligands to immobilize dioxo molydenum species by a reaction with MoO2(acac)2. This investigation comprises a thorough characterization of the process for building the immobilized molybdenum-Schiff base complexes, as well as the use of the obtained materials in 1-octene oxidation in the presence of organic hydroperoxides. These materials displayed high intrinsic catalytic activity in the epoxidation of 1-octene with organic hydroperoxides under a wide variety of conditions, although both the reaction solvent as well as the nature of the organic hydroperoxide, exerted a dramatic influence on the catalytic activity of these heterogeneous oxidation catalysts. Thus, whereas nonpolar solvents provided good epoxide yields with high efficiency in the use of the oxidant, polar solvents depressed the catalytic activity of the supported Mo-Schiff bases. These results have been ascribed to the competition with the solvent, when polar, for binding to the metal sites, thus avoiding the formation of the hydroperoxo-metal cycle and the epoxidation of the olefin. The catalysts presented here show good reusability with low catalytic activity decay after the first reuse. Full article
(This article belongs to the Special Issue Mesostructured Materials and Their Catalytic Applications)
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Open AccessArticle Pure and Fe-Doped Mesoporous Titania Catalyse the Oxidation of Acid Orange 7 by H2O2 under Different Illumination Conditions: Fe Doping Improves Photocatalytic Activity under Simulated Solar Light
Catalysts 2017, 7(7), 213; doi:10.3390/catal7070213
Received: 5 May 2017 / Revised: 11 July 2017 / Accepted: 11 July 2017 / Published: 18 July 2017
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Abstract
A sample of mesoporous TiO2 (MT, specific surface area = 150 m2·g−1) and two samples of MT containing 2.5 wt.% Fe were prepared by either direct synthesis doping (Fe2.5-MTd) or impregnation (Fe2.5-MTi). Commercial TiO2 (Degussa P25, specific
[...] Read more.
A sample of mesoporous TiO2 (MT, specific surface area = 150 m2·g−1) and two samples of MT containing 2.5 wt.% Fe were prepared by either direct synthesis doping (Fe2.5-MTd) or impregnation (Fe2.5-MTi). Commercial TiO2 (Degussa P25, specific surface area = 56 m2 g−1) was used both as a benchmark and as a support for impregnation with either 0.8 or 2.5 wt.% Fe (Fe0.80-IT and Fe2.5-IT). The powders were characterized by X-ray diffraction, N2 isotherms at −196 °C, Energy Dispersive X-ray (EDX) Spectroscopy, X-ray Photoelectron Spectroscopy (XPS), Diffuse Reflectance (DR) ultra-violet (UV)-Vis and Mössbauer spectroscopies. Degradation of Acid Orange 7 (AO7) by H2O2 was the test reaction: effects of dark-conditions versus both UV and simulated solar light irradiation were considered. In dark conditions, AO7 conversion was higher with MT than with Degussa P25, whereas Fe-containing samples were active in a (slow) Fenton-like reaction. Under UV light, MT was as active as Degussa P25, and Fe doping enhanced the photocatalytic activity of Fe2.5-MTd; Fe-impregnated samples were also active, likely due to the occurrence of a photo-Fenton process. Interestingly, the Fe2.5-MTd sample showed the best performance under solar light, confirming the positive effect of Fe doping by direct synthesis with respect to impregnation. Full article
(This article belongs to the Special Issue Mesostructured Materials and Their Catalytic Applications)
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Open AccessFeature PaperArticle Acidity-Reactivity Relationships in Catalytic Esterification over Ammonium Sulfate-Derived Sulfated Zirconia
Catalysts 2017, 7(7), 204; doi:10.3390/catal7070204
Received: 31 May 2017 / Revised: 29 June 2017 / Accepted: 29 June 2017 / Published: 5 July 2017
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Abstract
New insight was gained into the acidity-reactivity relationships of sulfated zirconia (SZ) catalysts prepared via (NH4)2SO4 impregnation of Zr(OH)4 for propanoic acid esterification with methanol. A family of systematically related SZs was characterized by bulk and surface
[...] Read more.
New insight was gained into the acidity-reactivity relationships of sulfated zirconia (SZ) catalysts prepared via (NH4)2SO4 impregnation of Zr(OH)4 for propanoic acid esterification with methanol. A family of systematically related SZs was characterized by bulk and surface analyses including XRD, XPS, TGA-MS, N2 porosimetry, temperature-programmed propylamine decomposition, and FTIR of adsorbed pyridine, as well as methylbutynol (MBOH) as a reactive probe molecule. Increasing surface sulfation induces a transition from amphoteric character for the parent zirconia and low S loadings <1.7 wt %, evidenced by MBOH conversion to 3-hydroxy-3-methyl-2-butanone, methylbutyne and acetone, with higher S loadings resulting in strong Brønsted-Lewis acid pairs upon completion of the sulfate monolayer, which favored MBOH conversion to prenal. Catalytic activity for propanoic acid esterification directly correlated with acid strength determined from propylamine decomposition, coincident with the formation of Brønsted-Lewis acid pairs identified by MBOH reactive titration. Monodispersed bisulfate species are likely responsible for superacidity at intermediate sulfur loadings. Full article
(This article belongs to the Special Issue Mesostructured Materials and Their Catalytic Applications)
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Open AccessArticle Highly Effective Dual Transition Metal Macrocycle Based Electrocatalyst with Macro-/Mesoporous Structures for Oxygen Reduction Reaction
Catalysts 2017, 7(7), 201; doi:10.3390/catal7070201
Received: 30 April 2017 / Revised: 16 June 2017 / Accepted: 19 June 2017 / Published: 30 June 2017
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Abstract
Metal macrocycle based non-noble metal electrocatalysts (NNMEs) with highly efficient oxygen reduction reaction (ORR) activity, good stability, and excellent resistance to the methanol cross-over effect have been regarded as one of the most important alternatives for Pt or Pt based alloys, which are
[...] Read more.
Metal macrocycle based non-noble metal electrocatalysts (NNMEs) with highly efficient oxygen reduction reaction (ORR) activity, good stability, and excellent resistance to the methanol cross-over effect have been regarded as one of the most important alternatives for Pt or Pt based alloys, which are widely used in fuel cells. However, the expensive price of most metal macrocycles hinder further investigation of such a family of NNMEs in large production for practical applications. Here, we introduce a simple strategy to synthesize metal macrocycle based porous carbon (MMPC) material with low cost and easy production of metal macrocycles (hemin (Hm) and vitamin B12 (VB12)) as raw materials by using a hard template of MgO. The pyrolysis of MMPC under the optimal temperature at 900 °C shows comparative ORR performance relative to commercial Pt/C, which could be attributed to the large surface area, macro-/mesoporous structure, the carbon layer encapsulating transition metal based oxides, as well as N-doped carbon species. In addition, MMPC (900) displays a better electrochemical property than 20 wt % Pt/C in terms of durability and tolerance to methanol in O2-saturated 0.1 M KOH media. Full article
(This article belongs to the Special Issue Mesostructured Materials and Their Catalytic Applications)
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Open AccessArticle Co3O4 Nanoparticle-Decorated N-Doped Mesoporous Carbon Nanofibers as an Efficient Catalyst for Oxygen Reduction Reaction
Catalysts 2017, 7(6), 189; doi:10.3390/catal7060189
Received: 20 April 2017 / Revised: 19 May 2017 / Accepted: 9 June 2017 / Published: 15 June 2017
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Abstract
A low cost, durable, and efficient electrocatalyst for oxygen reduction reactions (ORR) is essential for high-performance fuel cells. Here, we fabricated Co3O4 nanoparticles (NPs) anchored on N-doped mesoporous carbon nanofibers (Co3O4/NMCF) by electrospinning combined with the
[...] Read more.
A low cost, durable, and efficient electrocatalyst for oxygen reduction reactions (ORR) is essential for high-performance fuel cells. Here, we fabricated Co3O4 nanoparticles (NPs) anchored on N-doped mesoporous carbon nanofibers (Co3O4/NMCF) by electrospinning combined with the simple heat treatment. Within this composite, carbon nanofibers possess a mesoporous structure, contributed to obtain a high surface area, which can facilitate the infiltration of electrolyte. Moreover, this one-dimensional (1D) carbon nanofiber also acts as a 1D conductive channel, effectively improving the transmission of electrons. In addition, the doping of the N element with high content combined with homogenously distributed Co3O4 NPs can significantly enhance the ORR electrocatalytic activity. Benefiting from the advantages of material and structure, the Co3O4/NMCF catalyst favors a four electron transfer process in alkaline media, exhibiting good ORR electrocatalytic activity, and its durability is much better than that of commercial Pt/C. Full article
(This article belongs to the Special Issue Mesostructured Materials and Their Catalytic Applications)
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Open AccessArticle Post Synthesis of Aluminum Modified Mesoporous TUD-1 Materials and Their Application for FCC Diesel Hydrodesulfurization Catalysts
Catalysts 2017, 7(5), 141; doi:10.3390/catal7050141
Received: 22 February 2017 / Revised: 30 April 2017 / Accepted: 2 May 2017 / Published: 7 May 2017
PDF Full-text (5814 KB) | HTML Full-text | XML Full-text | Supplementary Files
Abstract
Post-synthesis methods are a promising technology and have received much attention. In this paper, a series of post-synthesis aluminum modified TUD-1 (PAT) materials with different Al contents were successfully prepared by using aluminum isopropoxide to be Al sources, then the as-synthesized materials were
[...] Read more.
Post-synthesis methods are a promising technology and have received much attention. In this paper, a series of post-synthesis aluminum modified TUD-1 (PAT) materials with different Al contents were successfully prepared by using aluminum isopropoxide to be Al sources, then the as-synthesized materials were adopted as support additives mixed with commercial γ-Al2O3 to prepare hydrodesulfurization (HDS) catalysts for FCC diesel. The supports and catalysts were analyzed using N2 adsorption-desorption, XRD, SEM, Py-IR, ICP, 27Al MAS NMR, UV-vis, H2-TPR and HRTEM techniques. The results of Py-IR and 27Al MAS NMR indicated that the addition of Al species could bring Lewis (L) and Brönsted (B) sites into Si-TUD-1, and that the material of PAT-3 had the highest total acidity sites and Brönsted acid sites among the series PAT composites. The HRTEM technique showed that, compared to the traditional catalyst NiMo/γ-Al2O3, the sulfided catalyst NiMo/APAT-3 had a relatively short length (3.2 nm) and suitable stacking number (2.5) of MoS2 slabs. The HDS efficiencies of all the catalysts were tested in a fixed bed micro-reactor with FCC diesel as feedstock. The catalytic results confirmed that the catalyst NiMo/APAT-3 possessed the highest HDS efficiency (97.0%), due to synergistic effects of advantageous properties such as higher acidity, moderate MSI, and relatively short length of the MoS2 slabs. Full article
(This article belongs to the Special Issue Mesostructured Materials and Their Catalytic Applications)
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Open AccessArticle Effect of Different Nano-Sized Silica Sols as Supports on the Structure and Properties of Cu/SiO2 for Hydrogenation of Dimethyl Oxalate
Catalysts 2017, 7(3), 75; doi:10.3390/catal7030075
Received: 6 January 2017 / Revised: 15 February 2017 / Accepted: 20 February 2017 / Published: 25 February 2017
PDF Full-text (2021 KB) | HTML Full-text | XML Full-text | Supplementary Files
Abstract
Cu/x-SiO2 catalysts with 4, 10, and 20 nm silica sols as supports was produced by ammonia evaporation method and characterized. Different nano-sized silica sols as supports significantly affected the structure and catalytic properties of the copper catalysts for ethylene glycol
[...] Read more.
Cu/x-SiO2 catalysts with 4, 10, and 20 nm silica sols as supports was produced by ammonia evaporation method and characterized. Different nano-sized silica sols as supports significantly affected the structure and catalytic properties of the copper catalysts for ethylene glycol synthesis from dimethyl oxalate. Compared with Cu/20-SiO2 and Cu/4-SiO2 catalysts, the catalytic performance and stability of Cu/10-SiO2 catalyst were greatly enhanced. The Cu/10-SiO2 catalyst showed 99.9% conversion with 94% EG selectivity and a lifetime of over 3080 h if it is calculated by industrial weight liquid hourly space velocity (WLHSV) of 0.5 h−1. The Cu/10-SiO2 catalyst has one of the longest lifetimes among the catalysts and is a good alternative catalyst for this reaction. Improvement in the catalytic performance and stability of Cu/10-SiO2 is attributed to the proper SBET, Dp and larger dispersion of copper. In addition, the supports of Cu/10-SiO2 catalyst have smaller particles than that of Cu/20-SiO2; thus, the migration and growth of copper species in catalysts are restrained during the reaction. Full article
(This article belongs to the Special Issue Mesostructured Materials and Their Catalytic Applications)
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