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Catalysts: Preparation, Catalytic Performance and Catalytic Reaction

A topical collection in Materials (ISSN 1996-1944). This collection belongs to the section "Catalytic Materials".

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Editors


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Guest Editor
Faculty of Chemical Sciences, University of Concepcion, Concepcion, Chile
Interests: heterogeneous catalysts; materials chemistry; catalysis

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Guest Editor
Department of Physical Chemistry, University of Concepcion, Concepcion, Chile

Topical Collection Information

Dear Colleagues,

Catalysts influence our daily lives and play a pivotal role in environmental protection. To be useful, catalysts must have a large activity (turnover frequency), selectivity (to a desired product), and durability (operational stability), properties not possible to find as a lucky circumstance. Therefore, to design a new catalyst, it is necessary to carry out a careful preparation and a deep characterization to understand catalytic performance, one of the earliest prioritie to be used in a given catalytic reaction.

The aim of this Special Issue is to cover the promising recent research and novel trends in the fields of the preparation of catalysts that reach the thermodynamic equilibrium faster with the lowest energy supply to be used in catalytic processes with academic and industrial interest. Full papers, short communications, and reviews in the field are welcome. Mini-reviews with an overview on the state-of-the-art with future perspectives and trends in this domain will be also considered.

The editors welcome contributions increasing the role of catalysts in environmental protection without any restrictions regarding the nature of the catalyst and the preparation method.

Prof. Gina Pecchi
Prof. Cristian H. Campos
Guest Editors

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Keywords

  • catalysis
  • catalytic performance
  • catalytic reaction
  • characterization
  • synthesis

Published Papers (27 papers)

2023

Jump to: 2022, 2021, 2020, 2019

16 pages, 6264 KiB  
Article
Effect of Potassium Doping on the Structural and Catalytic Properties of Co/MnOx Catalyst in the Steam Reforming of Ethanol
by Magdalena Greluk, Marek Rotko, Grzegorz Słowik, Sylwia Turczyniak-Surdacka, Gabriela Grzybek and Katarzyna Tyszczuk-Rotko
Materials 2023, 16(15), 5377; https://doi.org/10.3390/ma16155377 - 31 Jul 2023
Viewed by 787
Abstract
The promotional effect of potassium (~1.25 wt%) on a Co/MnOx catalyst was studied for samples prepared by the impregnation method in the steam reforming of ethanol (SRE) process at 420 °C for a H2O/EtOH molar ratio of 12/1. The catalysts [...] Read more.
The promotional effect of potassium (~1.25 wt%) on a Co/MnOx catalyst was studied for samples prepared by the impregnation method in the steam reforming of ethanol (SRE) process at 420 °C for a H2O/EtOH molar ratio of 12/1. The catalysts were characterized using physicochemical methods to study their textural, structural, and redox properties. The XRD studies revealed that, during the treatment of both cobalt-based catalysts under a hydrogen atmosphere at 500 °C, Co0 and MnO phases were formed by the reduction in Co3O4 and Mn2O3/Mn3O4 phases, respectively. Potassium doping significantly improved stability and ability for the C–C bond cleavage of the Co/MnOx catalyst. The enhancement of activity (at ~25%) and selectivity to hydrogen (at ca. 10%) and the C1 product, mainly carbon dioxide (at ~20%), of the Co/MnOx catalyst upon potassium doping was clarified by the alkali promoter’s impact on the reducibility of the cobalt and manganese oxides. The microscopic observations revealed that fibrous carbon deposits are present on the surface of Co/MnOx and KCo/MnOx catalysts after the SRE reaction and their formation is the main reason these catalysts deactivate under SRE conditions. However, carbon accumulation on the surface of the potassium-promoted catalyst was ca. 12% lower after 18 h of SRE reaction compared to the unpromoted sample. Full article
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15 pages, 6184 KiB  
Article
Synergistic Effect of P Doping and Mo-Ni-Based Heterostructure Electrocatalyst for Overall Water Splitting
by Feihong Jia, Xiangyu Zou, Xueling Wei, Weiwei Bao, Taotao Ai, Wenhu Li and Yuchen Guo
Materials 2023, 16(9), 3411; https://doi.org/10.3390/ma16093411 - 27 Apr 2023
Cited by 2 | Viewed by 1466
Abstract
Heterostructure construction and heteroatom doping are powerful strategies for enhancing the electrolytic efficiency of electrocatalysts for overall water splitting. Herein, we present a P-doped MoS2/Ni3S2 electrocatalyst on nickel foam (NF) prepared using a one-step hydrothermal method. The optimized [...] Read more.
Heterostructure construction and heteroatom doping are powerful strategies for enhancing the electrolytic efficiency of electrocatalysts for overall water splitting. Herein, we present a P-doped MoS2/Ni3S2 electrocatalyst on nickel foam (NF) prepared using a one-step hydrothermal method. The optimized P[0.9mM]-MoS2/Ni3S2@NF exhibits a cluster nanoflower-like morphology, which promotes the synergistic electrocatalytic effect of the heterostructures with abundant active centers, resulting in high catalytic activity for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in alkaline electrolyte. The electrode exhibits low overpotentials and Tafel slopes for the HER and OER. In addition, the catalyst electrode used in a two-electrode system for overall water splitting requires an ultralow voltage of 1.42 V at 10 mA·cm−2 and shows no obvious increase in current within 35 h, indicating excellent stability. Therefore, the combination of P doping and the heterostructure suggests a novel path to formulate high-performance electrocatalysts for overall water splitting. Full article
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18 pages, 6456 KiB  
Review
Supported Ionic Liquid Phase Catalysts Dedicated for Continuous Flow Synthesis
by Piotr Latos, Anna Wolny and Anna Chrobok
Materials 2023, 16(5), 2106; https://doi.org/10.3390/ma16052106 - 5 Mar 2023
Cited by 7 | Viewed by 2153
Abstract
Heterogeneous catalysis, although known for over a century, is constantly improved and plays a key role in solving the present problems in chemical technology. Thanks to the development of modern materials engineering, solid supports for catalytic phases having a highly developed surface are [...] Read more.
Heterogeneous catalysis, although known for over a century, is constantly improved and plays a key role in solving the present problems in chemical technology. Thanks to the development of modern materials engineering, solid supports for catalytic phases having a highly developed surface are available. Recently, continuous-flow synthesis started to be a key technology in the synthesis of high added value chemicals. These processes are more efficient, sustainable, safer and cheaper to operate. The most promising is the use of heterogeneous catalyst with column-type fixed-bed reactors. The advantages of the use of heterogeneous catalyst in continuous flow reactors are the physical separation of product and catalyst, as well as the reduction in inactivation and loss of the catalyst. However, the state-of-the-art use of heterogeneous catalysts in flow systems compared to homogenous ones remains still open. The lifetime of heterogeneous catalysts remains a significant hurdle to realise sustainable flow synthesis. The goal of this review article was to present a state of knowledge concerning the application of Supported Ionic Liquid Phase (SILP) catalysts dedicated for continuous flow synthesis. Full article
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13 pages, 5276 KiB  
Article
The Visible-Light-Driven Activity of Biochar-Doped TiO2 Photocatalysts in β-Blockers Removal from Water
by Agata Kowalczyk, Bożena Zgardzińska, Karol Osipiuk, Katarzyna Jędruchniewicz, Katarzyna Tyszczuk-Rotko, Magdalena Goździuk, Haitao Wang and Bożena Czech
Materials 2023, 16(3), 1094; https://doi.org/10.3390/ma16031094 - 27 Jan 2023
Cited by 2 | Viewed by 1548
Abstract
Water is the most important life-giving resource on earth. Nowadays, intensive growth of the world population has resulted in increased water consumption and the production of wastewater. Additionally, the presence of pharmaceuticals in treated conventional wastewater or even in the environment is strictly [...] Read more.
Water is the most important life-giving resource on earth. Nowadays, intensive growth of the world population has resulted in increased water consumption and the production of wastewater. Additionally, the presence of pharmaceuticals in treated conventional wastewater or even in the environment is strictly indicating that present techniques of wastewater treatment are not efficient enough and are not designed to remove such pollutants. Scarce water resources in the world are the main driving force for the innovation of novel techniques of water and wastewater treatment. Photocatalysis, as one of the advanced oxidation processes, enables the transformation of recalcitrant and toxic pollutants into CO2, water, and inorganic salts. In the present paper, the photocatalytic oxidation of β-blockers—metoprolol and propranolol—are described. For photocatalytic oxidation, novel TiO2 photocatalysts modified with biochar were used. Photocatalysts were prepared by sol-gel method and the effect of photocatalysts type, presence of inorganic ions, dissolved organic matter, and different water matrix was established. The results indicate that using only the decrease in the tested pollutant concentration is not effective enough in establishing the treatment method’s safety. There is a need to use additional testing such as ecotoxicity tests; however, the key parameter is the properly chosen tested organism. Full article
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2022

Jump to: 2023, 2021, 2020, 2019

13 pages, 4963 KiB  
Article
Modification of CeNi0.9Zr0.1O3 Perovskite Catalyst by Partially Substituting Yttrium with Zirconia in Dry Reforming of Methane
by Mahmud S. Lanre, Ahmed E. Abasaeed, Anis H. Fakeeha, Ahmed A. Ibrahim, Abdullah A. Alquraini, Salwa B. AlReshaidan and Ahmed S. Al-Fatesh
Materials 2022, 15(10), 3564; https://doi.org/10.3390/ma15103564 - 16 May 2022
Cited by 10 | Viewed by 1797
Abstract
Methane Dry Reforming is one of the means of producing syngas. CeNi0.9Zr0.1O3 catalyst and its modification with yttrium were investigated for CO2 reforming of methane. The experiment was performed at 800 °C to examine the effect of [...] Read more.
Methane Dry Reforming is one of the means of producing syngas. CeNi0.9Zr0.1O3 catalyst and its modification with yttrium were investigated for CO2 reforming of methane. The experiment was performed at 800 °C to examine the effect of yttrium loading on catalyst activity, stability, and H2/CO ratio. The catalyst activity increased with an increase in yttrium loading with CeNi0.9Zr0.01Y0.09O3 catalyst demonstrating the best activity with CH4 conversion >85% and CO2 conversion >90% while the stability increased with increases in zirconium loading. The specific surface area of samples ranged from 1–9 m2/g with a pore size of 12–29 nm. The samples all showed type IV isotherms. The XRD peaks confirmed the formation of a monoclinic phase of zirconium and the well-crystallized structure of the perovskite catalyst. The Temperature Program Reduction analysis (TPR) showed a peak at low-temperature region for the yttrium doped catalyst while the un-modified perovskite catalyst (CeNi0.9Zr0.1O3) showed a slight shift to a moderate temperature region in the TPR profile. The Thermogravimetric analysis (TGA) curve showed a weight loss step in the range of 500–700 °C, with CeNi0.9Zr0.1O3 having the least carbon with a weight loss of 20%. Full article
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2021

Jump to: 2023, 2022, 2020, 2019

16 pages, 3483 KiB  
Article
Outperformance in Acrylation: Supported D-Glucose-Based Ionic Liquid Phase on MWCNTs for Immobilized Lipase B from Candida antarctica as Catalytic System
by Anna Szelwicka, Karol Erfurt, Sebastian Jurczyk, Slawomir Boncel and Anna Chrobok
Materials 2021, 14(11), 3090; https://doi.org/10.3390/ma14113090 - 4 Jun 2021
Cited by 12 | Viewed by 2154
Abstract
This study presents a highly efficient method of a synthesis of n-butyl acrylate via esterification of acrylic acid and n-butanol in the presence of supported ionic liquid phase (SILP) biocatalyst consisting of the lipase B from Candida antarctica (CALB) and multi-walled [...] Read more.
This study presents a highly efficient method of a synthesis of n-butyl acrylate via esterification of acrylic acid and n-butanol in the presence of supported ionic liquid phase (SILP) biocatalyst consisting of the lipase B from Candida antarctica (CALB) and multi-walled carbon nanotubes (MWCNTs) modified by D-glucose-based ionic liquids. Favorable reaction conditions (acrylic acid: n-butanol molar ratio 1:2, cyclohexane as a solvent, biocatalyst 0.150 g per 1 mmol of acrylic acid, temperature 25 °C) allowed the achievement of a 99% yield of n-butyl acrylate in 24 h. Screening of various ionic liquids showed that the most promising result was obtained if N-(6-deoxy-1-O-methoxy-α-D-glucopyranosyl)-N,N,N-trimethylammonium bis-(trifluoromethylsulfonyl)imide ([N(CH3)3GlcOCH3][N(Tf)2]) was selected in order to modify the outer surface of MWCNTs. The final SILP biocatalyst–CNTs-[N(CH3)3GlcOCH3][N(Tf)2]-CALB contained 1.8 wt.% of IL and 4.2 wt.% of CALB. Application of the SILP biocatalyst led to the enhanced activity of CALB in comparison with the biocatalyst prepared via physical adsorption of CALB onto MWCNTs (CNTs-CALB), as well as with commercially available Novozyme 435. Thus, the crucial role of IL in the stabilization of biocatalysts was clearly demonstrated. In addition, a significant stability of the developed biocatalytic system was confirmed (three runs with a yield of ester over 90%). Full article
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2020

Jump to: 2023, 2022, 2021, 2019

15 pages, 3105 KiB  
Article
Fast and Efficient Piezo/Photocatalytic Removal of Methyl Orange Using SbSI Nanowires
by Krystian Mistewicz, Mirosława Kępińska, Marian Nowak, Agnieszka Sasiela, Maciej Zubko and Danuta Stróż
Materials 2020, 13(21), 4803; https://doi.org/10.3390/ma13214803 - 28 Oct 2020
Cited by 21 | Viewed by 3593
Abstract
Piezocatalysis is a novel method that can be applied for degradation of organic pollutants in wastewater. In this paper, ferroelectric nanowires of antimony sulfoiodide (SbSI) have been fabricated using a sonochemical method. Methyl orange (MO) was chosen as a typical pollutant, as it [...] Read more.
Piezocatalysis is a novel method that can be applied for degradation of organic pollutants in wastewater. In this paper, ferroelectric nanowires of antimony sulfoiodide (SbSI) have been fabricated using a sonochemical method. Methyl orange (MO) was chosen as a typical pollutant, as it is widely used as a dye in industry. An aqueous solution of MO at a concentration of 30 mg/L containing SbSI nanowires (6 g/L) was subjected to ultrasonic vibration. High degradation efficiency of 99.5% was achieved after an extremely short period of ultrasonic irradiation (40 s). The large reaction rate constant of 0.126(8) s−1 was determined for piezocatalytic MO decomposition. This rate constant is two orders of magnitude larger than values of reaction rate constants reported in the literature for the most efficient piezocatalysts. These promising experimental results have proved a great potential of SbSI nanowires for their application in environmental purification and renewable energy conversion. Full article
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12 pages, 3072 KiB  
Article
Study on Rh(I)/Ru(III) Bimetallic Catalyst Catalyzed Carbonylation of Methanol to Acetic Acid
by Shasha Zhang, Wenxin Ji, Ning Feng, Liping Lan, Yuanyuan Li and Yulong Ma
Materials 2020, 13(18), 4026; https://doi.org/10.3390/ma13184026 - 11 Sep 2020
Cited by 5 | Viewed by 3035
Abstract
In this study, a Rh(I)/Ru(III) catalyst with a bimetallic space structure was designed and synthesized. The interaction between the metals of the bimetallic catalyst and the structure of the bridged dimer can effectively reduce the steric hindrance effect and help speed up the [...] Read more.
In this study, a Rh(I)/Ru(III) catalyst with a bimetallic space structure was designed and synthesized. The interaction between the metals of the bimetallic catalyst and the structure of the bridged dimer can effectively reduce the steric hindrance effect and help speed up the reaction rate while ensuring the stability of the catalyst. X-ray photoelectron spectroscopy (XPS) results show that rhodium accepts electrons from chlorine, thereby increasing the electron-rich nature of rhodium and improving the catalytic activity. This promotes the nucleophilic reaction of the catalyst with methyl iodide and reduces the reaction energy barrier. The methanol carbonylation performance of the Rh/Ru catalyst was evaluated, and the results show that the conversion rate of methyl acetate and the yield of acetic acid are 96.0% under certain conditions. Furthermore, during the catalysis, no precipitate is formed and the amount of water is greatly reduced. It can be seen that the catalyst has good stability and activity. Full article
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13 pages, 3427 KiB  
Article
Synthesis and Performance of TiO2/Fly Ash Cenospheres as a Catalytic Film in a Novel Type of Periodic Air-Sparged Photocatalytic Reactor
by Witold Żukowski, Przemysław Migas, Dariusz Bradło and Piotr Dulian
Materials 2020, 13(7), 1691; https://doi.org/10.3390/ma13071691 - 4 Apr 2020
Cited by 6 | Viewed by 2913
Abstract
The results of a photocatalytic process performed in a new type of inclined, three-phase fluidised bed reactor with a periodic photocatalyst film are presented. These phases were fly ash cenospheres coated with TiO2, an aqueous solution of methylene blue and an [...] Read more.
The results of a photocatalytic process performed in a new type of inclined, three-phase fluidised bed reactor with a periodic photocatalyst film are presented. These phases were fly ash cenospheres coated with TiO2, an aqueous solution of methylene blue and an air stream passing from the bottom of the photoreactor. The cenospheres have a density lower than water and could thus form a catalytic film on a top irradiated window. The formed surface film is stable but is easy to break and be reproduced in a cyclic air-sparged process. Mixing was performed in either a cyclic or a continuous manner. From an operational point of view, the best variant of mixing was a 10 s air-sparge/10 s break with a 50% duty cycle, because it provided the same discolouration efficiency and reduced energy demand by 50% in comparison with the continuous mixing. Due to film formation, the proposed catalytic reactor enables a substantial reduction in the energy required for mixing while maintaining the desired degree of discolouration. Full article
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17 pages, 4834 KiB  
Article
Liquid Phase Hydrogenation of Pharmaceutical Interest Nitroarenes over Gold-Supported Alumina Nanowires Catalysts
by Krishnamoorthy Shanmugaraj, Tatiana M. Bustamante, Cristian H. Campos and Cecilia C. Torres
Materials 2020, 13(4), 925; https://doi.org/10.3390/ma13040925 - 19 Feb 2020
Cited by 11 | Viewed by 2650
Abstract
In this work, Au nanoparticles, supported in Al2O3 nanowires (ANW) modified with (3-aminopropyl)trimethoxysilane were synthetized, for their use as catalysts in the hydrogenation reaction of 4-(2-fluoro-4-nitrophenyl)-morpholine and 4-(4-nitrophenyl)morpholin-3-one. ANW was obtained by hydrothermal techniques and the metal was incorporated by [...] Read more.
In this work, Au nanoparticles, supported in Al2O3 nanowires (ANW) modified with (3-aminopropyl)trimethoxysilane were synthetized, for their use as catalysts in the hydrogenation reaction of 4-(2-fluoro-4-nitrophenyl)-morpholine and 4-(4-nitrophenyl)morpholin-3-one. ANW was obtained by hydrothermal techniques and the metal was incorporated by the reduction of the precursor with NaBH4 posterior to superficial modification. The catalysts were prepared at different metal loadings and were characterized by different techniques. The characterization revealed structured materials in the form of nanowires and a successful superficial modification. All catalysts show that Au is in a reduced state and the shape of the nanoparticles is spherical, with high metal dispersion and size distributions from 3.7 to 4.6 nm. The different systems supported in modified-ANW were active and selective in the hydrogenation reaction of both substrates, finding for all catalytic systems a selectivity of almost 100% to the aromatic amine. Catalytic data showed pseudo first-order kinetics with respect to the substrate for all experimental conditions used in this work. The solvent plays an important role in the activity and selectivity of the catalyst, where the highest efficiency and operational stability was achieved when ethanol was used as the solvent. Full article
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19 pages, 7058 KiB  
Article
Effect of Metal Content on Ethanol Decomposition over Ni-Co Catalysts Supported on La-Ce Oxides
by Harold R. Vergara, Maria H. Brijaldo, José J. Martinez, Hugo A. Rojas, José Pedraza, Fabio B. Passos, Luiz Pereira da Costa, Daniela Gonzalez-Vera and Paula Osorio-Vargas
Materials 2020, 13(3), 759; https://doi.org/10.3390/ma13030759 - 7 Feb 2020
Cited by 2 | Viewed by 2516
Abstract
The search for catalysts with features that can improve coke resistance and decrease byproduct formation is a current goal in H2 production from renewable sources. In this work, the effect of the presence of Ni nanoparticles over Co/La-Ce oxides on the ethanol [...] Read more.
The search for catalysts with features that can improve coke resistance and decrease byproduct formation is a current goal in H2 production from renewable sources. In this work, the effect of the presence of Ni nanoparticles over Co/La-Ce oxides on the ethanol decomposition reaction was studied. Catalysts were synthetized using as precursor a La0.8Ce0.2NixCo1-xO3 perovskite-type material to ensure a low segregation of phases and a high dispersion of metals. After reduction at 873 K, the perovskite structure was destroyed, and metal Co-Ni particles were supported over a lanthanum-cerium oxide. The materials were characterized by different techniques before and after reaction. Solids exhibited metal particle sizes between 5 and 15 nm demonstrating the advantages of the preparation method to obtain Ni-Co alloys. Although the results of adsorption of ethanol followed by diffuse reflectance infrared fourier transformed spectroscopy (DRIFTS) showed acetate species strongly adsorbed on the catalyst’s surface, the material (Ni0.7Co0.3/La0.8Ce0.2) with the lowest particle size was the most stable system leading to the lowest amount of carbon deposits during ethanol decomposition. This catalyst showed the better performance, with a higher ethanol conversion (98.4%) and hydrogen selectivity (75%). All catalysts exhibited carbonaceous deposits, which were an ordered and disordered carbon phase mixture. Full article
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17 pages, 1957 KiB  
Article
Thermal Modification Effect on Supported Cu-Based Activated Carbon Catalyst in Hydrogenolysis of Glycerol
by Juan Seguel, Rafael García, Ricardo José Chimentão, José Luis García-Fierro, I. Tyrone Ghampson, Néstor Escalona and Catherine Sepúlveda
Materials 2020, 13(3), 603; https://doi.org/10.3390/ma13030603 - 29 Jan 2020
Cited by 7 | Viewed by 3727
Abstract
Glycerol hydrogenolysis to 1,2-propanediol (1,2-PDO) was performed over activated carbon supported copper-based catalysts. The catalysts were prepared by impregnation using a pristine carbon support and thermally-treated carbon supports (450, 600, 750, and 1000 °C). The final hydrogen adsorption capacity, porous structure, and total [...] Read more.
Glycerol hydrogenolysis to 1,2-propanediol (1,2-PDO) was performed over activated carbon supported copper-based catalysts. The catalysts were prepared by impregnation using a pristine carbon support and thermally-treated carbon supports (450, 600, 750, and 1000 °C). The final hydrogen adsorption capacity, porous structure, and total acidity of the catalysts were found to be important descriptors to understand catalytic performance. Oxygen surface groups on the support controlled copper dispersion by modifying acidic and adsorption properties. The amount of oxygen species of thermally modified carbon supports was also found to be a function of its specific surface area. Carbon supports with high specific surface areas contained large amount of oxygen surface species, inducing homogeneous distribution of Cu species on the carbon support during impregnation. The oxygen surface groups likely acted as anchorage centers, whereby the more stable oxygen surface groups after the reduction treatment produced an increase in the interaction of the copper species with the carbon support, and determined catalytic performances. Full article
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13 pages, 5413 KiB  
Article
A Fenton-Like Nanocatalyst Based on Easily Separated Magnetic Nanorings for Oxidation and Degradation of Dye Pollutant
by Xiaonan Li, Jinghua Li, Weilu Shi, Jianfeng Bao and Xianyuan Yang
Materials 2020, 13(2), 332; https://doi.org/10.3390/ma13020332 - 11 Jan 2020
Cited by 15 | Viewed by 3060
Abstract
In this study, uniform Fe3O4 magnetic nanorings (Fe3O4-MNRs) were prepared through a simple hydrothermal method. The morphology, magnetic properties, and structure of the product were characterized by transmission electron microscope (TEM), scanning electron microscope (SEM), high [...] Read more.
In this study, uniform Fe3O4 magnetic nanorings (Fe3O4-MNRs) were prepared through a simple hydrothermal method. The morphology, magnetic properties, and structure of the product were characterized by transmission electron microscope (TEM), scanning electron microscope (SEM), high resolution transmission electron microscopy (HRTEM), vibrating sample magnetometer (VSM), X-ray powder diffraction (XRD), and X-ray photoelectron spectroscopy (XPS), respectively. The Fe3O4-MNRs were used as Fenton-like catalysts in the presence of hydrogen peroxide (H2O2) and showed excellent Fenton-catalytic activity for degradation of organic dyes such as Methylene blue (MB), Rhodamine B (RhB), and Bromophenol blue (BPB). Furthermore, the obtained Fe3O4-MNRs could be recycled after used for several times and still remained in a relative high activity and could rapidly be separated from the reaction medium using a magnet without considerable loss. All results reveal that Fe3O4-MNRs have potential for the treatment of dyes pollutants. Full article
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16 pages, 3201 KiB  
Article
The Effect of the ZrO2 Loading in SiO2@ZrO2-CaO Catalysts for Transesterification Reaction
by Daniela Salinas, Sichem Guerrero, Cristian H. Campos, Tatiana M. Bustamante and Gina Pecchi
Materials 2020, 13(1), 221; https://doi.org/10.3390/ma13010221 - 4 Jan 2020
Cited by 6 | Viewed by 3631
Abstract
The effect of the ZrO2 loading was studied on spherical SiO2@ZrO2-CaO structures synthetized by a simple route that combines the Stöber and sol-gel methods. The texture of these materials was determined using SBET by N2 adsorption, [...] Read more.
The effect of the ZrO2 loading was studied on spherical SiO2@ZrO2-CaO structures synthetized by a simple route that combines the Stöber and sol-gel methods. The texture of these materials was determined using SBET by N2 adsorption, where the increment in SiO2 spheres’ surface areas was reached with the incorporation of ZrO2. Combined the characterization techniques of using different alcoholic dissolutions of zirconium (VI) butoxide 0.04 M, 0.06 M, and 0.08 M, we obtained SiO2@ZrO2 materials with 5.7, 20.2, and 25.2 wt % of Zr. Transmission electron microscopy (TEM) analysis also uncovered the shape and reproducibility of the SiO2 spheres. The presence of Zr and Ca in the core–shell was also determined by TEM. X-ray diffraction (XRD) profiles showed that the c-ZrO2 phase changed in to m-ZrO2 by incorporating calcium, which was confirmed by Raman spectroscopy. The purity of the SiO2 spheres, as well as the presence of Zr and Ca in the core–shell, was assessed by the Fourier transform infrared (FTIR) method. CO2 temperature programmed desorption (TPD-CO2) measurements confirmed the increment in the amount of the basic sites and strength of these basic sites due to calcium incorporation. The catalyst reuse in FAME production from canola oil transesterification allowed confirmation that these calcium core@shell catalysts turn out to be actives and stables for this reaction. Full article
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2019

Jump to: 2023, 2022, 2021, 2020

12 pages, 2536 KiB  
Article
Magnetic Fe3O4@SiO2–Pt and Fe3O4@SiO2–Pt@SiO2 Structures for HDN of Indole
by Robinson Dinamarca, Verónica Valles, Brenda Ledesma, Cristian H. Campos, Gina Pecchi and Andrea Beltramone
Materials 2019, 12(23), 3878; https://doi.org/10.3390/ma12233878 - 24 Nov 2019
Cited by 3 | Viewed by 3781
Abstract
The effect of a second porous SiO2 shell in the activity and selectivity of the Fe3O4@SiO2–Pt catalyst in the hydrodenitrogenation of indole is reported. The double Fe3O4@SiO2–Pt@SiO2 structure was [...] Read more.
The effect of a second porous SiO2 shell in the activity and selectivity of the Fe3O4@SiO2–Pt catalyst in the hydrodenitrogenation of indole is reported. The double Fe3O4@SiO2–Pt@SiO2 structure was prepared by coating Fe3O4 nanoparticles with tetraethyl orthosilicate (TEOS) with a further impregnation of 1.0 wt.% of Pt on the (3-aminopropyl)triethoxysilane functionalized Fe3O4@SiO2 structures. The second porous SiO2 shell, obtained by using a hexadecyltrimethylammonium bromide (CTAB) template, covered the Fe3O4@SiO2–Pt catalyst with a well-defined and narrow pore-sized distribution. The full characterization by TEM, inductively coupled plasma-optical emission spectroscopy (ICP-OES), XRD, and N2 adsorption isotherm at 77 K and vibrating sample magnetometry (VSM) of the catalysts indicates homogeneous core@shell structures with a controlled nano-size of metallic Pt. A significant effect of the double SiO2 shell in the catalytic performance was demonstrated by both a higher activity to eliminate the nitrogen atom of the indole molecule present in model liquid fuel and the improvement of the catalytic stability reaching four consecutive reaction cycles with only a slight conversion level decrease. Full article
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15 pages, 3109 KiB  
Article
Impact of Support (MCF, ZrO2, ZSM-5) on the Efficiency of Ni Catalyst in High-Temperature Conversion of Lignocellulosic Biomass to Hydrogen-Rich Gas
by Jacek Grams, Robert Ryczkowski, Karolina Chałupka, Izabela Sobczak, Izabela Rzeźnicka and Kamila Przybysz
Materials 2019, 12(22), 3792; https://doi.org/10.3390/ma12223792 - 19 Nov 2019
Cited by 10 | Viewed by 2886
Abstract
The main objective of this work was to evaluate an impact of a support on the efficiency of nickel catalysts in the high-temperature conversion of lignocellulosic biomass to hydrogen-rich gas. The most important parameters influencing catalytic performance of the catalysts were identified. The [...] Read more.
The main objective of this work was to evaluate an impact of a support on the efficiency of nickel catalysts in the high-temperature conversion of lignocellulosic biomass to hydrogen-rich gas. The most important parameters influencing catalytic performance of the catalysts were identified. The properties of three materials (ZSM-5, ZrO2, and MCF (mesostructured cellular foam)) used as a support differing in surface acidity, surface area, pore structure, ability to interact with an active phase, and resistance to coking, have been studied. The results revealed that Ni/MCF, characterized by large pore size and pore volume, low acidity, small NiO crystallites size, and moderate interaction with the active phase, is the most efficient among studied catalysts, while an application of Ni on ZSM-5 support with high-acidity was not beneficial. The results suggest that structure of the support, in particular larger pore size and a better contact between an active phase and reaction intermediates, play an important role in the formation of gaseous products during thermal decomposition of lignocellulosic feedstock. On the other hand, high acidity of the support did not increase the formation of large amounts of hydrogen-rich gaseous products. Full article
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16 pages, 5946 KiB  
Article
Low Temperature NH3-SCR over Mn-Ce Oxides Supported on MCM-41 from Diatomite
by Mingxuan Ma, Xiaoyu Ma, Suping Cui, Tingting Liu, Yingliang Tian and Yali Wang
Materials 2019, 12(22), 3654; https://doi.org/10.3390/ma12223654 - 6 Nov 2019
Cited by 11 | Viewed by 2616
Abstract
A series of MCM-41 molecular sieves with different molar ratio of template to silicon were synthesized through hydrothermal synthesis method by using cetyltrimethylammonium bromide (CTAB) as the template, diatomite as the silicon source. By using impregnation method, the Mn-Ce/MCM-41 SCR molecular sieve-based catalysts [...] Read more.
A series of MCM-41 molecular sieves with different molar ratio of template to silicon were synthesized through hydrothermal synthesis method by using cetyltrimethylammonium bromide (CTAB) as the template, diatomite as the silicon source. By using impregnation method, the Mn-Ce/MCM-41 SCR molecular sieve-based catalysts were prepared. The results observed that when the molar ratio of template to silicon was 0.2:1, the MCM-41 as catalyst carrier has the highest surface area and largest pore volume, it also presented typically ordered hexagonal arrays of uniform channels. The denitration catalytic material based on this carrier has a high number of Lewis acidic sites, and the denitration efficiency can reach more than 93%. Full article
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17 pages, 6959 KiB  
Article
Novel Route to Obtain Carbon Self-Doped TiO2 Mesoporous Nanoparticles as Efficient Photocatalysts for Environmental Remediation Processes under Visible Light
by Pablo A. Ochoa Rodríguez, Tamara B. Benzaquén, Gina A. Pecchi, Sandra G. Casuscelli, Verónica R. Elías and Griselda A. Eimer
Materials 2019, 12(20), 3349; https://doi.org/10.3390/ma12203349 - 14 Oct 2019
Cited by 8 | Viewed by 2817
Abstract
Titanium dioxide materials were synthesized using two different methods. The samples were characterized by X-ray diffraction (XRD), UV–Visible diffusion reflectance spectroscopy (UV-Vis DR), Raman spectroscopy, N2 adsorption/desorption, scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), transmission electron spectroscopy (TEM) and X-ray photoelectron [...] Read more.
Titanium dioxide materials were synthesized using two different methods. The samples were characterized by X-ray diffraction (XRD), UV–Visible diffusion reflectance spectroscopy (UV-Vis DR), Raman spectroscopy, N2 adsorption/desorption, scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), transmission electron spectroscopy (TEM) and X-ray photoelectron spectroscopy (XPS). Although both kind of materials were found to have mesoporous structure and anatase crystalline phase, one of them was obtained from a synthesis method that does not involve the use of surfactants, and therefore, does not require calcination at high temperatures. This implies that the synthesized solid was self-doped with carbon species, coming only from the same source used for titanium. Then, the relationship between the presence of these species, the final calcination temperature, and the photocatalytic activity of the solids was studied in terms of the degradation and mineralization of an Acid Orange 7 aqueous solution, under visible radiation. A photosensitizing effect caused by the non-metal presence, that allows the solid to extend its absorption range, was found. Hence, a novel route to prepare C-modified photoactive mesoporous TiO2, simpler and cheaper, where neither a template nor an external carbon source is used, could be performed. Full article
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20 pages, 8226 KiB  
Article
Mesoporous Palladium N,N’-Bis(3-Allylsalicylidene)o-Phenylenediamine-Methyl Acrylate Resins as Heterogeneous Catalysts for the Heck Coupling Reaction
by Claudio Mella, Cecilia C. Torres, Gina Pecchi and Cristian H. Campos
Materials 2019, 12(16), 2612; https://doi.org/10.3390/ma12162612 - 16 Aug 2019
Cited by 1 | Viewed by 3054
Abstract
Palladium N,N’-bis(3-allylsalicylidene)o-phenylenediamine complex (PdAS) immobilized onto mesoporous polymeric methyl acrylate (MA) based resins (PdAS(x)-MA, x = 1, 2, 5, or 10 wt.%) were successfully prepared as heterogeneous catalysts for the Heck reaction. The catalysts were synthesized via radical suspension polymerization using PdAS as [...] Read more.
Palladium N,N’-bis(3-allylsalicylidene)o-phenylenediamine complex (PdAS) immobilized onto mesoporous polymeric methyl acrylate (MA) based resins (PdAS(x)-MA, x = 1, 2, 5, or 10 wt.%) were successfully prepared as heterogeneous catalysts for the Heck reaction. The catalysts were synthesized via radical suspension polymerization using PdAS as a metal chelate monomer, divinylbenzene and MA as co-monomers. The effect of the PdAS(x) content on the physicochemical properties of the resins is also reported. The catalysts were characterized by using a range of analytical techniques. The large surface area (>580 m2·g−1) and thermal stability (up to 250 °C) of the PdAS(x)-MA materials allows their application as catalysts in the C–C coupling reaction between iodobenzene and MA in the presence of trimethylamine at 120 °C using DMF as the solvent. The PdAS(10)-MA catalyst exhibited the highest catalytic performance with no significant catalytic loss being observed after five reuses, thereby indicating excellent catalyst stability in the reaction medium. Full article
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16 pages, 4283 KiB  
Article
Effect of SO2 on the Selective Catalytic Reduction of NOx over V2O5-CeO2/TiO2-ZrO2 Catalysts
by Yaping Zhang, Peng Wu, Ke Zhuang, Kai Shen, Sheng Wang and Wanqiu Guo
Materials 2019, 12(16), 2534; https://doi.org/10.3390/ma12162534 - 9 Aug 2019
Cited by 13 | Viewed by 2782
Abstract
The effect of SO2 on the selective catalytic reduction of NOx by NH3 over V2O5-0.2CeO2/TiO2-ZrO2 catalysts was studied through catalytic activity tests and various characterization methods, like Brunner−Emmet−Teller (BET) surface measurement, [...] Read more.
The effect of SO2 on the selective catalytic reduction of NOx by NH3 over V2O5-0.2CeO2/TiO2-ZrO2 catalysts was studied through catalytic activity tests and various characterization methods, like Brunner−Emmet−Teller (BET) surface measurement, X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray fluorescence (XRF), hydrogen temperature-programmed desorption (H2-TPR), X-ray photoelectron spectroscopy (XPS) and in situ diffused reflectance infrared Fourier transform spectroscopy (DRIFTS). The results showed that the catalyst exhibited superior SO2 resistance when the volume fraction of SO2 was below 0.02%. As the SO2 concentration further increased, the NOx conversion exhibited some degree of decline but could restore to the original level when stopping feeding SO2. The deactivation of the catalyst caused by water in the flue gas was reversible. However, when 10% H2O was introduced together with 0.06% SO2, the NOx conversion was rapidly reduced and became unrecoverable. Characterizations indicated that the specific surface area of the deactivated catalyst was significantly reduced and the redox ability was weakened, which was highly responsible for the decrease of the catalytic activity. XPS results showed that more Ce3+ was generated in the case of reacting with SO2. In situ DRIFTS results confirmed that the adsorption capacity of SO2 was enhanced obviously in the presence of O2, while the SO2 considerably refrained the adsorption of NH3. The adsorption of NOx was strengthened by SO2 to some extent. In addition, NH3 adsorption was improved after pre-adsorbed by SO2 + O2, indicating that the Ce3+ and more oxygen vacancy were produced. Full article
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16 pages, 9198 KiB  
Article
Synthesis of Petal-Like MnO2 Nanosheets on Hollow Fe3O4 Nanospheres for Heterogeneous Photocatalysis of Biotreated Papermaking Effluent
by Yangliu Du, Fuqiang Li, Yecan Peng, Shaowu Jia, Lei Lan, Jinghong Zhou and Shuangfei Wang
Materials 2019, 12(15), 2346; https://doi.org/10.3390/ma12152346 - 24 Jul 2019
Cited by 3 | Viewed by 3155
Abstract
Owing to the implementation of increasingly stringent water conservation policies and regulations, the pulp and paper mill industry must make increased efforts to meet the limits for pollutant emissions. The primary pretreatment and secondary biochemical treatment methods used currently generally fail to meet [...] Read more.
Owing to the implementation of increasingly stringent water conservation policies and regulations, the pulp and paper mill industry must make increased efforts to meet the limits for pollutant emissions. The primary pretreatment and secondary biochemical treatment methods used currently generally fail to meet the country-specific environmental regulations, and the wastewater must be processed further even after being subjected to secondary biochemical treatments. In this work, we synthesized Fe3O4/MnO2 nanocomposites (FMNs) with a flower-like structure for use in the heterogeneous photocatalytic treatment of biotreated papermaking wastewater. FMNs1.25, which were formed using a KMnO4/Fe3O4 molar ratio of 1.25, could be separated readily using an external magnetic field and exhibited higher photocatalytic activity than those of the other samples as well as MnO2 and Fe3O4. The effects of various experimental parameters on the photocatalytic activity of FMNs1.25, including the initial pH of the wastewater and the catalyst dosage, were determined. The common chemical oxygen demand (CODCr) reduction rate in the case of this sample reached 56.58% within 120 min at a pH of 3, the CODCr of effluent after treatment was 52.10 mg/L. Further, even under neutral conditions, the CODCr of the treated effluent was below the current limit for discharge in China. Moreover, the nanocomposites exhibited good recyclability, and their catalytic activity did not decrease significantly even after five usage cycles. This study should serve as a platform for the fabrication of effective photocatalysts for the advanced treatment of biotreated papermaking effluent and refractory organic wastewater. Full article
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11 pages, 3900 KiB  
Article
Cyclodehydration of 1,4-butanediol over Zr-Al Catalysts: Effect of Reaction Medium
by Kuo-Tseng Li and Kuan-Wen Chen
Materials 2019, 12(13), 2092; https://doi.org/10.3390/ma12132092 - 28 Jun 2019
Cited by 5 | Viewed by 3989
Abstract
The conversion of 1,4-butanediol (BDO) to tetrahydrofuran (THF) in aqueous phase is desirable because BDO production technology is shifting to bio-based aqueous fermentation routes. In this study, liquid-phase cyclodehydration of BDO to THF was studied in two reaction media (pure BDO and aqueous [...] Read more.
The conversion of 1,4-butanediol (BDO) to tetrahydrofuran (THF) in aqueous phase is desirable because BDO production technology is shifting to bio-based aqueous fermentation routes. In this study, liquid-phase cyclodehydration of BDO to THF was studied in two reaction media (pure BDO and aqueous BDO feeds) at 200–240 °C using ZrO2-Al2O3 (ZA) mixed oxides, which were made with a co-precipitation method and were characterized with XRD, BET, SEM/EDX, pyridine and n-butylamine adsorptions. The maximum acidity and the largest surface area occurred at Zr/Al atomic ratios of 1/1 (ZA11) and 1/3 (ZA13), respectively. The reaction exhibited pseudo-first-order; aqueous BDO feed had much greater rate constant than pure BDO feed, ascribed to the acidic properties of adsorbed water molecules (coordinated to surface metal cations) for the former case. For pure BDO feed, linear relation was observed between rate constant and catalyst acidity, and ZA11 reached a THF yield of 90.1% at 240 °C. With aqueous BDO feed, rate constant increased linearly with increasing surface area and ZA13 reached a THF yield of 97.1% at 220 °C. The change of optimum catalyst composition with reaction medium suggests that active sites for catalyzing BDO cyclodehydration changed with the reaction environment. Full article
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26 pages, 5883 KiB  
Review
Recent Advances in Carbonaceous Photocatalysts with Enhanced Photocatalytic Performances: A Mini Review
by Jianlong Ge, Yifan Zhang and Soo-Jin Park
Materials 2019, 12(12), 1916; https://doi.org/10.3390/ma12121916 - 13 Jun 2019
Cited by 95 | Viewed by 5898
Abstract
Photocatalytic processes based on various semiconductors have been widely utilized in different applications, with great potential for use in environmental pollution remediation and sustainable energy generation. However, critical issues, including low light adsorption capability, wide energy bandgap, and unsatisfactory physicochemical stability still seriously [...] Read more.
Photocatalytic processes based on various semiconductors have been widely utilized in different applications, with great potential for use in environmental pollution remediation and sustainable energy generation. However, critical issues, including low light adsorption capability, wide energy bandgap, and unsatisfactory physicochemical stability still seriously limit the practical applications of photocatalysts. As a solution, the introduction of carbonaceous materials with different structures and properties into a photocatalyst system to further increase the activity has attracted much research attention. This mini review surveys the related literatures and highlights recent progress in the development of carbonaceous photocatalysts, which include various metal semiconductors with activated carbon, carbon dots, carbon nanotubes/nanofibers, graphene, fullerene, and carbon sponges/aerogels. Moreover, graphitic carbon nitride is also discussed as a carbon-rich and metal-free photocatalyst. The recently developed synthesis strategies and proposed mechanisms underlying the photocatalytic activity enhancement for different applications are summarized and discussed. Finally, ongoing challenges and the developmental direction for carbonaceous photocatalysts are proposed. Full article
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12 pages, 5839 KiB  
Article
Influence of Nature Support on Methane and CO2 Conversion in a Dry Reforming Reaction over Nickel-Supported Catalysts
by Anis Hamza Fakeeha, Samsudeen Olajide Kasim, Ahmed Aidid Ibrahim, Ahmed Elhag Abasaeed and Ahmed Sadeq Al-Fatesh
Materials 2019, 12(11), 1777; https://doi.org/10.3390/ma12111777 - 31 May 2019
Cited by 25 | Viewed by 3992
Abstract
A promising method to reduce global warming has been methane reforming with CO2, as it combines two greenhouse gases to obtain useful products. In this study, Ni-supported catalysts were synthesized using the wet impregnation method to obtain 5%Ni/Al2O3 [...] Read more.
A promising method to reduce global warming has been methane reforming with CO2, as it combines two greenhouse gases to obtain useful products. In this study, Ni-supported catalysts were synthesized using the wet impregnation method to obtain 5%Ni/Al2O3(SA-5239), 5%Ni/Al2O3(SA-6175), 5%Ni/SiO2, 5%Ni/MCM41, and 5%Ni/SBA15. The catalysts were tested in dry reforming of methane at 700 °C, 1 atm, and a space velocity of 39,000 mL/gcat h, to study the interaction of Ni with the supports, and evaluation was based on CH4 and CO2 conversions. 5%Ni/Al2O3(SA-6175) and 5%Ni/SiO2 gave the highest conversion of CH4 (78 and 75%, respectively) and CO2 (84 and 82%, respectively). The catalysts were characterized by some techniques. Ni phases were identified by X-ray diffraction patterns. Brunauer–Emmett–Teller analysis showed different surface areas of the catalysts with the least being 4 m2/g and the highest 668 m2/g belonging to 5%Ni/Al2O3(SA-5239) and 5%Ni/SBA15, respectively. The reduction profiles revealed weak NiO-supports interaction for 5%Ni/Al2O3(SA-5239), 5%Ni/MCM41, and 5%Ni/SBA15; while strong interaction was observed in 5%Ni/Al2O3(SA-6175) and 5%Ni/SiO2. The 5%Ni/Al2O3(SA-6175) and 5%Ni/SiO2 were close with respect to performance; however, the former had a higher amount of carbon deposit, which is mostly graphitic, according to the conducted thermal analysis. Carbon deposits on 5%Ni/SiO2 were mainly atomic in nature. Full article
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13 pages, 4776 KiB  
Article
Highly Active AuCu-Based Catalysts for Acetylene Hydrochlorination Prepared Using Organic Aqua Regia
by Haihua He, Jia Zhao, Bolin Wang, Yuxue Yue, Gangfeng Sheng, Qingtao Wang, Lu Yu, Zhong-Ting Hu and Xiaonian Li
Materials 2019, 12(8), 1310; https://doi.org/10.3390/ma12081310 - 22 Apr 2019
Cited by 8 | Viewed by 3726
Abstract
Development of a sustainable process for designing and synthesising an active and stable catalyst for hydrochlorination of acetylene is challenging, yet crucial, for industrial vinyl chloride monomer (VCM) production. Herein, direct synthesis of bimetallic AuCu catalysts using organic aqua regia (OAR) preparation methods [...] Read more.
Development of a sustainable process for designing and synthesising an active and stable catalyst for hydrochlorination of acetylene is challenging, yet crucial, for industrial vinyl chloride monomer (VCM) production. Herein, direct synthesis of bimetallic AuCu catalysts using organic aqua regia (OAR) preparation methods was investigated. In comparison with conventional aqua regia (AR), bimetallic AuCu catalysts synthesised from OAR exhibit enhanced activity and stability. After careful characterisation of the catalyst samples using X-ray diffraction patterns (XRD), Scanning transmission electron microscopy (STEM), X-ray photoelectron spectroscopy (XPS), and Temperature-programmed desorption (TPD), this observation was justified for the following reasons: 1) the existence of sulphur and nitrogen atoms stabilised the cationic Au active sites, and 2) OAR helped to sustain the function of the Cu promotor by stabilising it. Advanced understanding on the importance of promoter stability has unveiled new perspectives for this research area. Full article
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14 pages, 4415 KiB  
Article
The Influence of Si/Al Ratios on Adsorption and Desorption Characterizations of Pd/Beta Served as Cold-Start Catalysts
by Ming Jiang, Jun Wang, Jianqiang Wang and Meiqing Shen
Materials 2019, 12(7), 1045; https://doi.org/10.3390/ma12071045 - 29 Mar 2019
Cited by 17 | Viewed by 3180
Abstract
The majority of NOx is exhausted during the cold-start period for the low temperature of vehicle emissions, which can be solved by using Pd/zeolite catalysts to trap NOx at low temperature and release NOx at a high temperature that must [...] Read more.
The majority of NOx is exhausted during the cold-start period for the low temperature of vehicle emissions, which can be solved by using Pd/zeolite catalysts to trap NOx at low temperature and release NOx at a high temperature that must be higher than the operating temperature of selective catalytic reduction catalysts (SCR). In this work, several Pd/Beta catalysts were prepared to identify the influence of Si/Al ratios on NO and C3H6 adsorption and desorption characterizations. The physicochemical properties were identified using N2 physical adsorption, Fourier Transform Infrared Spectroscopy (FT-IR), transmission electron microscopy (TEM), X-ray photo electron spectroscopy (XPS), and Na+ titration, while the adsorption and desorption characterizations were investigated by catalyst evaluation. The results indicated that the amount of dispersed Pd ions, the main active sites for NO and C3H6 adsorption, decreased with the increase of Si/Al ratios. Besides this, the intensity of Brønsted and Lewis acid decreased with the increase of Si/Al ratios, which also led to the decrease of NO and C3H6 adsorption amounts. Therefore, Pd dispersion and the acidic properties of Pd/Beta together determined the adsorption ability of NO and C3H6. Moreover, lower Si/Al ratios resulted in the formation of an additional dispersed Pd cationic species, Pd(OH)+, from which adsorbed NO released at a much lower temperature. Finally, an optimum Si/Al ratio of Pd/Beta was found at around 55 due to the balanced performance between the adsorption amounts and desorption temperature. Full article
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16 pages, 2723 KiB  
Article
Combustion Synthesis of Non-Precious CuO-CeO2 Nanocrystalline Catalysts with Enhanced Catalytic Activity for Methane Oxidation
by Abdallah F. Zedan and Amina S. AlJaber
Materials 2019, 12(6), 878; https://doi.org/10.3390/ma12060878 - 15 Mar 2019
Cited by 23 | Viewed by 3825
Abstract
In this study, xCuO-CeO2 mixed oxide catalysts (Cu weight ratio x = 1.5, 3, 4.5, 6 and 15 wt.%) were prepared using solution combustion synthesis (SCS) and their catalytic activities towards the methane (CH4) oxidation reaction were studied. The combustion [...] Read more.
In this study, xCuO-CeO2 mixed oxide catalysts (Cu weight ratio x = 1.5, 3, 4.5, 6 and 15 wt.%) were prepared using solution combustion synthesis (SCS) and their catalytic activities towards the methane (CH4) oxidation reaction were studied. The combustion synthesis of the pure CeO2 and the CuO-CeO2 solid solution catalysts was performed using copper and/or cerium nitrate salt as an oxidizer and citric acid as a fuel. A variety of standard techniques, including scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDX), X-ray diffraction (XRD), thermo-gravimetric analysis (TGA), X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy were employed to reveal the microstructural, crystal, thermal and electronic properties that may affect the performance of CH4 oxidation. The CuO subphase was detected in the prepared solid solution and confirmed with XRD and Raman spectroscopy, as indicated by the XRD peaks at diffraction angles of 35.3° and 38.5° and the Ag Raman mode at 289 cm−1, which are characteristics of tenorite CuO. A profound influence of Cu content was evident, not only affecting the structural and electronic properties of the catalysts, but also the performance of catalysts in the CH4 oxidation. The presence of Cu in the CeO2 lattice obviously promoted its catalytic activity for CH4 catalytic oxidation. Among the prepared catalysts, the 6% CuO-CeO2 catalyst demonstrated the highest performance, with T50 = 502 °C and T80 = 556 °C, an activity that is associated with the availability of a fine porous structure and the enhanced surface area of this catalyst. The results demonstrate that nanocrystalline copper-ceria mixed oxide catalysts could serve as an inexpensive and active material for CH4 combustion. Full article
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