Special Issue "Non-critical Element- and Non-critical Loading of Critical Element-Based Catalysts for Environmentally Friendly Catalytic Processes"

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

Deadline for manuscript submissions: 31 January 2021.

Special Issue Editor

Prof. Dr. Maria Olea, FRSC
Website1 Website2
Guest Editor
1. School of Science and Engineering, Teesside University, Middlesbrough, Tees Valley, TS1 3BA, UK
2. Institute for Catalysis, Hokkaido University, Kita 21, Nishi 10, Kita-ku, Sapporo, Hokkaido, Japan
Interests: heterogeneous catalysis applied to environmentally friendly processes; scale-up of catalysts; scale-down of reactors (microreactors)

Special Issue Information

Dear colleagues,

Modern society has an ever-increasing demand for environmentally friendly catalytic processes, either for clean manufacturing of chemicals or for renewable energy production, elimination of environmental pollutants from air, water and soil or for waste conversion into useful products. Although noble metal-based catalysts have proven to be very efficient for all these environmentally friendly catalytic processes, due to their scarcity and cost, alternative catalytic technologies are being developed based on either their non-critical loadings or non-critical elements. This Special Issue is focused on “Non-critical Element and Non-critical Loading of Critical Element-Based Catalysts for Environmentally Friendly Catalytic Processes” with the aim to present the most recent and innovative scientific results in this field, regarding all aspects of design and formulation, preparation, characterisation, scale-up and engineering aspects for commercially applications.

Prof. Dr. Maria Olea, FRSC
Guest Editor

Manuscript Submission Information

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

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2000 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

  • Non-critical element catalysts
  • Non-critical loading of critical element catalysts, preparation
  • characterisation
  • scale-up
  • catalytic reactors and microreactors
  • design
  • formulation

Published Papers (3 papers)

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Research

Open AccessArticle
Catalytic Degradation of Chitosan by Supported Heteropoly Acids in Heterogeneous Systems
Catalysts 2020, 10(9), 1078; https://doi.org/10.3390/catal10091078 - 18 Sep 2020
Abstract
Several kinds of composite materials with phosphotungstic acid (PTA) as the catalyst were prepared with activated carbon as support, and their structures were characterized. According to the Box–Behnken central combination principle, the mathematical model of the heterogeneous system is established. Based on the [...] Read more.
Several kinds of composite materials with phosphotungstic acid (PTA) as the catalyst were prepared with activated carbon as support, and their structures were characterized. According to the Box–Behnken central combination principle, the mathematical model of the heterogeneous system is established. Based on the single-factor experiments, the reaction temperature, the reaction time, the amount of hydrogen peroxide and the loading capacity of PTA were selected as the influencing factors to study the catalyzed oxidation of hydrogen peroxide and degradation of high molecular weight chitosan. The results of IR showed that the catalyst had a Keggin structure. The results of the mercury intrusion test showed that the pore structure of the supported PTA catalyst did not change significantly, and with the increase of PTA loading, the porosity and pore volume decreased regularly, which indicated that PTA molecules had been absorbed and filled into the pore of activated carbon. The results of Response Surface Design (RSD) showed that the optimum reaction conditions of supported PTA catalysts for oxidative degradation of high molecular weight chitosan by hydrogen peroxide were as follows: reaction temperature was 70 ℃, reaction time was 3.0 h, the ratio of hydrogen peroxide to chitosan was 2.4 and the catalyst loading was 30%. Under these conditions, the yield and molecular weight of water-soluble chitosan were 62.8% and 1290 Da, respectively. The supported PTA catalyst maintained high catalytic activity after three reuses, which indicated that the supported PTA catalyst had excellent catalytic activity and stable performance compared with the PTA catalyst. Full article
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Open AccessArticle
Micro-Reactor System for Complete Oxidation of Volatile Organic Compounds
Catalysts 2020, 10(8), 846; https://doi.org/10.3390/catal10080846 - 28 Jul 2020
Abstract
Based on previous Computational Fluid Dynamics (CFD) design results, an 11 channel microreactor of dimensions (0.5 mm × 0.5 mm × 100 mm) (width × depth × length) and optimal manifold geometry was fabricated, coated with a newly-developed Au/SBA-15 catalyst and then integrated [...] Read more.
Based on previous Computational Fluid Dynamics (CFD) design results, an 11 channel microreactor of dimensions (0.5 mm × 0.5 mm × 100 mm) (width × depth × length) and optimal manifold geometry was fabricated, coated with a newly-developed Au/SBA-15 catalyst and then integrated in an experimental rig specifically built for this research. Propane (as model volatile organic compound) oxidation experiments were conducted at three different flow velocities, 12.5, 15.4 and 17.5 m/min, respectively, at six temperatures, 150, 200, 225, 250, 275, and 300 °C, respectively. The catalyst was prepared by one-pot sol-gel synthesis of SBA-15 with MPTMS (3-mercaptopropyl-trimethoxy-silane) before loading with HAuCl4 gold precursor and then characterized by SEM/EDX, TEM and wide angle XRD. A novel catalyst coating technique was developed, using airbrush (0.3 nozzle) to spray a catalyst slurry into the microchannels that produced a thin, firm and uniform layer of Au/SBA-15 catalyst coating inside the microreactor. The experimental measurements revealed that propane conversion increased as the flow feed rates decreased and increased with increasing temperatures in the reactor. For the built microreactor and for the flows and temperatures set, the combustion of propane was possible with measurable conversions and reasonable reactor stability, the performance of the catalyst appeared to be central to the satisfactory operation of the reactor. Full article
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Open AccessArticle
The Distinctive Effects of Glucose-Derived Carbon on the Performance of Ni-Based Catalysts in Methane Dry Reforming
Catalysts 2020, 10(1), 21; https://doi.org/10.3390/catal10010021 - 23 Dec 2019
Abstract
This study aimed to investigate the effect of carbon derived from glucose (C) on the physicochemical characteristics and catalytic activity of Ni, supported over SiO2, ZSM-5, and TiO2 in methane dry reforming. Among the Ni catalysts without C, Ni/SiO2 [...] Read more.
This study aimed to investigate the effect of carbon derived from glucose (C) on the physicochemical characteristics and catalytic activity of Ni, supported over SiO2, ZSM-5, and TiO2 in methane dry reforming. Among the Ni catalysts without C, Ni/SiO2 exhibited the highest CH4-CO2 conversion and stability at all experimented temperatures. On the other hand, the C-incorporated catalysts prepared by glucose impregnation, followed by pyrolysis, showed dissimilar performances. C improved the stability of Ni/SiO2 in the reforming at 650 °C and 750 °C and increased the CH4 and CO2 conversion to the level close to the thermodynamic equilibrium at 850 °C. However, this element did not substantially affect the activity of Ni/ZSM-5 and exerted a retarding effect on Ni/TiO2. Characterizations with H2-TPD, XRD, EXAFS, and STEM-EDS revealed that the different influences of C by the supports were attributed to the extent of metal dispersion and metal-support interaction. Full article
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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.

Title: Active and coking resistant Ni/SBA-15 catalysts for low temperature dry reforming of methane
Author: Prof. Dr. Maria Olea
Abstract: In recent years CO2 reforming of methane has attracted great interest as it produces high CO/H2 ratio syngas suitable for the synthesis of higher hydrocarbons and oxygenated derivatives, since it is a way for disposing and recycling two greenhouse gases with high environmental impact, CH4 and CO2, and because it is regarded as a potential route to store and transmit energy due to its strong endothermic effect. Along with noble metals, all of the group VIII metals, except for osmium, have been studied for catalytic CO2 reforming of methane. It was found that the catalytic activity of Ni, though lower than those of Ru and Rh, was higher than the catalytic activity of Pt and Pd. Although noble metals have been proved to be insensitive to coke, the high cost and restricted availability limit their use in this process. It is therefore valuable to develop stable Ni-based catalysts. In this contribution, we show how their activity and coking resistivity is greatly related to the size and dispersion of Ni particles. Well-dispersed Ni nanoparticles were achieved by multistep impregnation on a mesoporous silica support, namely SBA-15, obtained through a sol-gel method, using acetate as nickel precursor and keeping the Ni loading between 5 wt% and 11 wt%. Significant catalytic activity was obtained at temperatures as low as 450°C, temperature well below their deactivation temperature, i.e., 700°C. For the pre-reduced samples complete CO2 conversion was obtained around 680°C. As such, their deactivation by sintering and coke formation was prevented. To the best of our knowledge, no Ni-based catalysts with complete CO2 conversion at temperatures lower than 800°C were reported so far.

Title: Adsorption and Desorption of deuterium on Ni2P (0001) surface
Authors: Hiroko Ariga-Miwa1,2, Takeshi Miyamoto1,2, Satoru Takakusagi1,2, , and Kiyotaka Asakura1,2*
Affiliation: 1 Department of Quantum Science and Engineering, Graduate School of Engineering, Hokkaido University, Kita21 Nishi10, Kita-ku, Sapporo 001-0021, Japan
2 Institute of Catalysis (ICAT), Hokkaido University, Kita21 Nishi10, Kita-ku, Sapporo 001-0021, Japan
Abstract: Ni2P has drawn much attention because of its high activity for hydrogen transfer reactions with fossil fuels or biomass materials as well as its high rate in the hydrogen evolution reaction in the electrolysis of water   In order to understand the interaction of hydrogen with the Ni2P surface, the surface adsorption properties of hydrogen(or D2) were investigated on a Ni2P(0001)-1x1 single crystal by D2-TPD (temperature-programmed desorption), photoemission electron microscopy, and density functional theory (DFT) calculations.  It was found that molecular D2 did not adsorb dissociatively on the Ni2P(0001) surface even at high temperatures, while atomic D was strongly adsorbed on the same surface.   The D2-TPD profile showed the highest desorption peak of D23) at 480 K which was accompanied with PD3 desorption, and which was higher than that observed on the Ni(111)-1x1 surface.  The desorption energy of the D23) peak was 1.99±0.07 and 1.53±0.08 eV at coverages of about 0.20 and 0.44 monolayers, respectively.  The peaks were assigned to desorption from the topmost P of the Ni3P_P structure by DFT calculations.   Both surface P and Ni could be adsorption sites for D and this might be related to the high activity of Ni2P in hydrotreatment reactions and the hydrogen evolution reaction. 

Title: Micro-reactor system for complete oxidation of volatile organic compounds
Authors: Sunday Odiba1, Maria Olea1,2, Emmanuel Iro1, Paul Russell1, Takehiko Sasaki3, Simon Hodgson1, Adam Adgar1
Affiliations: 1   Teesside University, School of Science, Engineering and Design, Borough Road, Middlesbrough TS1 3BX, UK;     
2   Hokkaido University, Institute for Catalysis, Sapporo, Kita 21, Nishi 10, Kita-ku, Sapporo, Hokkaido, Japan, 001-0021
3 The University of Tokyo, Graduate School of Frontier Sciences, Department of Complexity Science and Engineering, 5 Chome-1-5 Kashiwanoha, Kashiwa, Chiba 277-0882; Japan
Abstract: Propane oxidation as a model molecule for VOC was studied in an 11 channel microreactor of dimensions (0.5 mm X 0.5mm X 100mm) (width X depth X length). CFD module of COMSOL Multiphysics was used to set up an optimum geometry for a microreactor system. In terms of the Fluid Dynamics, the model attempted to find an optimum geometry based on the flow profile across a channel. The optimised manifold geometry of the reactor was constructed.  A novel catalyst coating techniques was developed, using airbrush (0.3 nozzle) to spray catalyst slurry into the microchannels that produce a thin, firm and uniform layer of Au/SBA-15 catalyst coating inside the channels of the microreactor.
Experiments for a range of conditions with Au/SBA-15 catalyst coated on the inside of the microreactor tubes/channels were carried out and complete oxidation of propane was investigated for different reactant flow rates and temperatures using the optimum geometry already established.
The experimental measurement revealed that propane conversion increased at lower feed rates and increased with increasing temperatures in the reactor. It did appear that for the microreactor constructed and the flows and temperatures set a combustion of the propane was possible with measurable conversions and reasonable reactor stability, the performance of the catalyst appeared to be central to the satisfactory operation of the reactor.
Keywords: Microreactor, CFD, VOCs, Au/SBA-15 catalyst, propane, complete oxidation, catalyst coating

Title: The distinctive effects of glucose-derived carbon on the performance of Ni-based catalysts in methane dry reforming
Authors: UPM. Ashik1, Shusaku Asano1, Shinji Kudo1, Doan Pham Minh4, Srinivas Appari5, Einaga Hisahiro2, Jun-ichiro Hayashi1,3*
Affiliations: 1     Institute for Materials Chemistry and Engineering, Kyushu University, 6-1, Kasuga Koen, Kasuga 816-8580, Japan
2     Faculty of Engineering Sciences, Kyushu University, 6-1, Kasuga Koen, Kasuga, Fukuoka 816-8580, Japan
3     Transdisciplinary Research and Education Center of Green Technology, Kyushu University, Kasuga 816-8580, Japan
4     Université de Toulouse, IMT Mines Albi, RAPSODEE CNRS UMR-5302, Albi cedex 09, France
5   Department of Chemical Engineering, Birla Institute of Technology and Science, Pilani, Rajasthan 333 031, India
Abstract: This study aims to investigate the effect of carbon derived from glucose (C) on the physicochemical characteristics and catalytic activity of Ni supported over SiO2, ZSM-5, and TiO2 in methane dry reforming. Among the Ni catalysts without C, Ni/SiO2 exhibited the highest CH4-CO2 conversion and stability at all experimented temperatures. On the other hand, the C-incorporated catalysts prepared by glucose impregnation, followed by pyrolysis, showed dissimilar performances. C improved the stability of Ni/SiO2 in the reforming at 650 °C and 750 °C and increased the CH4 and CO2 conversion to the level close to the thermodynamic equilibrium at 850 °C. However, this element did not substantially affect the activity of Ni/ZSM-5 and exerted a retarding effect on Ni/TiO2. Characterizations with H2-TPD, XRD, EXAFS, and TEM-EDS revealed that the different influences of C by the supports were attributed to the extent of metal dispersion and metal–support interaction.
Keywords: methane dry reforming; syngas; Ni-catalyst; ZSM-5; SiO2, TiO2; glucose derived carbon; metal dispersion

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