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Catalysis for the Production of Sustainable Fuels and Chemicals
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Catalysis for the Production of Sustainable Fuels and Chemicals

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

Deadline for manuscript submissions: closed (30 November 2019) | Viewed by 72373

Printed Edition Available!
A printed edition of this Special Issue is available here.

Special Issue Editors

Prof. Dr. Flora T. T. Ng

E-Mail Website
Guest Editor
Department of Chemical Engineering, University of Waterloo, 200 University Avenue West, Waterloo, ON N2L 3G1, Canada
Interests: solid acid catalysis; clean fuels; chemicals from biomass; process intensification; esterification; transesterification; hydrogenolysis; desulfurization; hydrocracking
Prof. Dr. Ajay K. Dalai

E-Mail Website
Guest Editor
Department of Chemical and Biological Engineering, University of Saskatchewan, Saskatoon, SK S7N 5A9, Canada
Interests: hydro-deoxygenation; hydrogenolysis; hydrogenation; biomass; esterification and transesterification; pyrolysis; gasification; hydrothermal treatment; Fischer-Tropsch synthesis; hydroprocessing
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Green-house gas emissions and environmental concerns have led to recent research in the use of renewable feedstocks derived from biomass, waste oils, and fats as a source of fuels and chemicals. However, these feedstocks contain a large amount of oxygen functional groups. Processing these feedstocks generally requires esterification and transesterification, deoxygenation, hydrogenation, hydrogenolysis, aldol condensation and cracking reactions. In addition, the bio-oils produced through pyrolysis and hydrothermal treatment are treated through catalytic processes for producing clean fuels. In addition, syngas produced through gasification of biomass is converted to liquid fuels. The main focus of this Special Issue is to solicit recent advances in the catalytic processing of these renewable feedstocks to produce sustainable fuels and chemicals.

Prof. Flora T. T. Ng
Prof. Ajay K. Dalai
Guest Editors

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 2700 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 Fuels and Chemicals
  • Hydrogenolysis
  • Deoxygenation
  • Esterification and Transesterification
  • Hydroprocessing
  • Cracking
  • Pyrolysis
  • Gasification
  • Hydrothermal Treatment Biomass
  • Bio-oil and Fats
  • Catalysis

Published Papers (16 papers)

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Editorial

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3 pages, 144 KiB  
Editorial
Catalysis for the Production of Sustainable Fuels and Chemicals
by Flora T. T. Ng and Ajay K. Dalai
Catalysts 2020, 10(4), 388; https://doi.org/10.3390/catal10040388 - 02 Apr 2020
Cited by 7 | Viewed by 1860
Abstract
The emission of green-house gases and environmental concerns have led to recent research in the use of renewable feedstocks derived from biomass, waste oils and fats as a source for fuels and chemicals [...] Full article
(This article belongs to the Special Issue Catalysis for the Production of Sustainable Fuels and Chemicals)

Research

Jump to: Editorial

21 pages, 3692 KiB  
Article
Catalytic Pyrolysis of Aliphatic Carboxylic Acids into Symmetric Ketones over Ceria-Based Catalysts: Kinetics, Isotope Effect and Mechanism
by Tetiana Kulik, Borys Palianytsia and Mats Larsson
Catalysts 2020, 10(2), 179; https://doi.org/10.3390/catal10020179 - 03 Feb 2020
Cited by 19 | Viewed by 4106
Abstract
Ketonization is a promising way for upgrading bio-derived carboxylic acids from pyrolysis bio-oils, waste oils, and fats to produce high value-added chemicals and biofuels. Therefore, an understanding of its mechanism can help to carry out the catalytic pyrolysis of biomass more efficiently. Here [...] Read more.
Ketonization is a promising way for upgrading bio-derived carboxylic acids from pyrolysis bio-oils, waste oils, and fats to produce high value-added chemicals and biofuels. Therefore, an understanding of its mechanism can help to carry out the catalytic pyrolysis of biomass more efficiently. Here we show that temperature-programmed desorption mass spectrometry (TPD-MS) together with linear free energy relationships (LFERs) can be used to identify catalytic pyrolysis mechanisms. We report the kinetics of the catalytic pyrolysis of deuterated acetic acid and a reaction series of linear and branched fatty acids into symmetric ketones on the surfaces of ceria-based oxides. A structure–reactivity correlation between Taft’s steric substituent constants Es* and activation energies of ketonization indicates that this reaction is the sterically controlled reaction. Surface D3-n-acetates transform into deuterated acetone isotopomers with different yield, rate, E≠, and deuterium kinetic isotope effect (DKIE). The obtained values of inverse DKIE together with the structure–reactivity correlation support a concerted mechanism over ceria-based catalysts. These results demonstrate that analysis of Taft’s correlations and using simple equation for estimation of DKIE from TPD-MS data are promising approaches for the study of catalytic pyrolysis mechanisms on a semi-quantitative level. Full article
(This article belongs to the Special Issue Catalysis for the Production of Sustainable Fuels and Chemicals)
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13 pages, 6511 KiB  
Article
Enhancement of HDO Activity of MoP/SiO2 Catalyst in Physical Mixture with Alumina or Zeolites
by Ivan V. Shamanaev, Irina V. Deliy, Evgeny Yu. Gerasimov, Vera P. Pakharukova and Galina A. Bukhtiyarova
Catalysts 2020, 10(1), 45; https://doi.org/10.3390/catal10010045 - 31 Dec 2019
Cited by 12 | Viewed by 2699
Abstract
Catalytic properties of physical mixture of MoP/SiO2 catalyst with SiC, γ-Al2O3, SAPO-11 and zeolite β have been compared in hydrodeoxygenation of methyl palmitate (MP). MoP/SiO2 catalyst (11.5 wt% of Mo, Mo/P = 1) was synthesized using TPR [...] Read more.
Catalytic properties of physical mixture of MoP/SiO2 catalyst with SiC, γ-Al2O3, SAPO-11 and zeolite β have been compared in hydrodeoxygenation of methyl palmitate (MP). MoP/SiO2 catalyst (11.5 wt% of Mo, Mo/P = 1) was synthesized using TPR method and characterized with N2 physisorption, elemental analysis, H2-TPR, XRD and TEM. Trickle-bed reactor was used for catalytic properties investigation at hydrogen pressure of 3 MPa, and 290 °C. The conversions of MP and overall oxygen-containing compounds have been increased significantly (from 59 to about 100%) when γ-Al2O3 or zeolite materials were used instead of inert SiC. MP can be converted to palmitic acid through acid-catalyzed hydrolysis along with metal-catalyzed hydrogenolysis, and as a consequence the addition of material possessing acid sites to MoP/SiO2 catalyst could lead to acceleration of MP hydrodeoxygenation through acid-catalyzed reactions. Isomerization and cracking of alkane were observed over the physical mixture of MoP/SiO2 with zeolites, but the selectivity of MP conversion trough the HDO reaction route is remained on the high level exceeding 90%. Full article
(This article belongs to the Special Issue Catalysis for the Production of Sustainable Fuels and Chemicals)
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13 pages, 1786 KiB  
Article
Catalytic Decomposition of Oleic Acid to Fuels and Chemicals: Roles of Catalyst Acidity and Basicity on Product Distribution and Reaction Pathways
by Wanpeng Hu, Hui Wang, Hongfei Lin, Ying Zheng, Siauw Ng, Manlin Shi, Ying Zhao and Ruoqian Xu
Catalysts 2019, 9(12), 1063; https://doi.org/10.3390/catal9121063 - 13 Dec 2019
Cited by 11 | Viewed by 4050
Abstract
The roles of catalyst acidity and basicity playing in catalytic conversion of oleic acid were studied in a fixed-bed micro-reactor at atmospheric pressure. The chemical compositions of the petroleum-like products were obtained and the reaction pathways of different catalysts are discussed. The metal [...] Read more.
The roles of catalyst acidity and basicity playing in catalytic conversion of oleic acid were studied in a fixed-bed micro-reactor at atmospheric pressure. The chemical compositions of the petroleum-like products were obtained and the reaction pathways of different catalysts are discussed. The metal oxides are suitable for upgrading oleic acid into organic liquid products (OLPs). Over 98% oxygen was removed when CaO, MgO, and TiO2 were implemented, whereas a minimum oxygen removal lower than 20% was obtained by using quartz. The oxygen removal was 73% by alumina; however, the light oil yield (to feed) and the valuable product yield received were the highest in all investigated catalysts. The hydrocarbons in OLPs, overwhelmingly presenting in the product, were found to be alkenes and cycloalkenes, followed by saturated hydrocarbons, and then aromatics lower than 4%. For Lewis acidic catalysts, higher acidity of the catalyst is beneficial to deoxygenation but also secondary cracking. CaO has higher dehydrogenation capability than MgO does. Full article
(This article belongs to the Special Issue Catalysis for the Production of Sustainable Fuels and Chemicals)
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21 pages, 1984 KiB  
Article
Hydroprocessing of Oleic Acid for Production of Jet-Fuel Range Hydrocarbons over Cu and FeCu Catalysts
by Afees A. Ayandiran, Philip E. Boahene, Ajay K. Dalai and Yongfeng Hu
Catalysts 2019, 9(12), 1051; https://doi.org/10.3390/catal9121051 - 11 Dec 2019
Cited by 8 | Viewed by 3512
Abstract
In the present study, a series of monometallic Cu/SiO2-Al2O3 catalysts exhibited immense potential in the hydroprocessing of oleic acid to produce jet-fuel range hydrocarbons. The synergistic effect of Fe on the monometallic Cu/SiO2-Al2O3 [...] Read more.
In the present study, a series of monometallic Cu/SiO2-Al2O3 catalysts exhibited immense potential in the hydroprocessing of oleic acid to produce jet-fuel range hydrocarbons. The synergistic effect of Fe on the monometallic Cu/SiO2-Al2O3 catalysts of variable Cu loadings (5–15 wt%) was ascertained by varying Fe contents in the range of 1–5 wt% on the optimized 13% Cu/SiO2-Al2O3 catalyst. At 340 °C and 2.07 MPa H2 pressure, the jet-fuel range hydrocarbons yield and selectivities of 51.8% and 53.8%, respectively, were recorded for the Fe(3)-Cu(13)/SiO2-Al2O3 catalyst. To investigate the influence of acidity of support on the cracking of oleic acid, ZSM-5 (Zeolite Socony Mobil–5) and HZSM-5(Protonated Zeolite Socony Mobil–5)-supported 3% Fe-13% Cu were also evaluated at 300–340 °C and 2.07 MPa H2 pressure. Extensive techniques including N2 sorption analysis, pyridine- Fourier Transform Infrared Spectroscopy (Pyridine-FTIR), X-ray Diffraction (XRD), X-ray Photoelectron Spectroscopy (XPS), and H2-Temperature Programmed Reduction (H2-TPR) analyses were used to characterize the materials. XPS analysis revealed the existence of Cu1+ phase in the Fe(3)-Cu(13)/SiO2-Al2O3 catalyst, while Cu metal was predominant in both the ZSM-5 and HZSM-5-supported FeCu catalysts. The lowest crystallite size of Fe(3)-Cu(13)/SiO2-Al2O3 was confirmed by XRD, indicating high metal dispersion and corroborated by the weakest metal–support interaction revealed from the TPR profile of this catalyst. CO chemisorption also confirmed high metal dispersion (8.4%) for the Fe(3)-Cu(13)/SiO2-Al2O3 catalyst. The lowest and mildest Brønsted/Lewis acid sites ratio was recorded from the pyridine–FTIR analysis for this catalyst. The highest jet-fuel range hydrocarbons yield of 59.5% and 73.6% selectivity were recorded for the Fe(3)-Cu(13)/SiO2-Al2O3 catalyst evaluated at 300 °C and 2.07 MPa H2 pressure, which can be attributed to its desirable textural properties, high oxophilic iron content, high metal dispersion and mild Brønsted acid sites present in this catalyst. Full article
(This article belongs to the Special Issue Catalysis for the Production of Sustainable Fuels and Chemicals)
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17 pages, 5006 KiB  
Article
Atomic Layer Deposition ZnO Over-Coated Cu/SiO2 Catalysts for Methanol Synthesis from CO2 Hydrogenation
by Jinglin Gao, Philip Effah Boahene, Yongfeng Hu, Ajay Dalai and Hui Wang
Catalysts 2019, 9(11), 922; https://doi.org/10.3390/catal9110922 - 06 Nov 2019
Cited by 14 | Viewed by 3443
Abstract
Cu-ZnO-based catalysts are of importance for CO2 utilization to synthesize methanol. However, the mechanisms of CO2 activation, the split of the C=O double bond, and the formation of C-H and O-H bonds are still debatable. To understand this mechanism and to [...] Read more.
Cu-ZnO-based catalysts are of importance for CO2 utilization to synthesize methanol. However, the mechanisms of CO2 activation, the split of the C=O double bond, and the formation of C-H and O-H bonds are still debatable. To understand this mechanism and to improve the selectivity of methanol formation, the combination of strong electronic adsorption (SEA) and atomic layer deposition (ALD) was used to form catalysts with Cu nanoparticles surrounded by a non-uniform ZnO layer, uniform atomic layer of ZnO, or multiple layers of ZnO on porous SiO2. N2 adsorption, H2 temperature-programmed reduction (H2-TPR) X-ray diffraction (XRD), transmission electron microscope (TEM), energy-dispersive X-ray spectroscopy (EDX), CO-chemisorption, CO2 temperature-programmed desorption (CO2-TPD), X-ray adsorption near edge structure (XANES), and extended X-ray absorption fine structure (EXAFS) were used to characterize the catalysts. The catalyst activity was correlated to the number of metallic sites. The catalyst of 5 wt% Cu over-coated with a single atomic layer of ZnO exhibited higher methanol selectivity. This catalyst has comparatively more metallic sites (smaller Cu particles with good distribution) and basic site (uniform ZnO layer) formation, and a stronger interaction between them, which provided necessary synergy for the CO2 activation and hydrogenation to form methanol. Full article
(This article belongs to the Special Issue Catalysis for the Production of Sustainable Fuels and Chemicals)
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17 pages, 2617 KiB  
Article
Effect of Surface Composition and Structure of the Mesoporous Ni/KIT-6 Catalyst on Catalytic Hydrodeoxygenation Performance
by Xianming Zhang, Shuang Chen, Fengjiao Wang, Lidan Deng, Jianmin Ren, Zhaojie Jiao and Guilin Zhou
Catalysts 2019, 9(11), 889; https://doi.org/10.3390/catal9110889 - 25 Oct 2019
Cited by 10 | Viewed by 3232
Abstract
A series of Ni/KIT6 catalyst precursors with 25 wt.% Ni loading amount were reduced in H2 at 400, 450, 500, and 550 °C, respectively. The studied catalysts were investigated by XRD, Quasi in-situ XPS, BET, TEM, and H2-TPD/Ranalysis methods. It [...] Read more.
A series of Ni/KIT6 catalyst precursors with 25 wt.% Ni loading amount were reduced in H2 at 400, 450, 500, and 550 °C, respectively. The studied catalysts were investigated by XRD, Quasi in-situ XPS, BET, TEM, and H2-TPD/Ranalysis methods. It was found that reduction temperature is an important factor affecting the hydrodeoxygenation (HDO) performance of the studied catalysts because of the Strong Metal Support Interaction Effect (SMSI). The reduction temperature influences mainly the content of active components, crystal size, and the abilityfor adsorbing and activating H2. The developed pore structure and large specific surface area of the KIT-6 support favored the Ni dispersion. The RT450 catalyst, which was prepared in H2 atmosphere at 450 °C, has the best HDO performance. Ethyl acetate can be completely transformed and maintain 96.8% ethane selectivity and 3.2% methane selectivity at 300 °C. The calculated apparent activation energies of the prepared catalysts increased in the following order: RT550 > RT400 > RT500 > RT450. Full article
(This article belongs to the Special Issue Catalysis for the Production of Sustainable Fuels and Chemicals)
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20 pages, 6126 KiB  
Article
Artificial Intelligence Modelling Approach for the Prediction of CO-Rich Hydrogen Production Rate from Methane Dry Reforming
by Bamidele Victor Ayodele, Siti Indati Mustapa, May Ali Alsaffar and Chin Kui Cheng
Catalysts 2019, 9(9), 738; https://doi.org/10.3390/catal9090738 - 31 Aug 2019
Cited by 20 | Viewed by 3902
Abstract
This study investigates the applicability of the Leven–Marquardt algorithm, Bayesian regularization, and a scaled conjugate gradient algorithm as training algorithms for an artificial neural network (ANN) predictively modeling the rate of CO and H2 production by methane dry reforming over a Co/Pr [...] Read more.
This study investigates the applicability of the Leven–Marquardt algorithm, Bayesian regularization, and a scaled conjugate gradient algorithm as training algorithms for an artificial neural network (ANN) predictively modeling the rate of CO and H2 production by methane dry reforming over a Co/Pr2O3 catalyst. The dataset employed for the ANN modeling was obtained using a central composite experimental design. The input parameters consisted of CH4 partial pressure, CO2 partial pressure, and reaction temperature, while the target parameters included the rate of CO and H2 production. A neural network architecture of 3 13 2, 3 15 2, and 3 15 2 representing the input layer, hidden neuron layer, and target (output) layer were employed for the Leven–Marquardt, Bayesian regularization, and scaled conjugate gradient training algorithms, respectively. The ANN training with each of the algorithms resulted in an accurate prediction of the rate of CO and H2 production. The best prediction was, however, obtained using the Bayesian regularization algorithm with the lowest standard error of estimates (SEE). The high values of coefficient of determination (R2 > 0.9) obtained from the parity plots are an indication that the predicted rates of CO and H2 production were strongly correlated with the observed values. Full article
(This article belongs to the Special Issue Catalysis for the Production of Sustainable Fuels and Chemicals)
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14 pages, 2256 KiB  
Article
The Effects of Catalyst Support and Temperature on the Hydrotreating of Waste Cooking Oil (WCO) over CoMo Sulfided Catalysts
by Hui Wang, Kyle Rogers, Haiping Zhang, Guoliang Li, Jianglong Pu, Haoxuan Zheng, Hongfei Lin, Ying Zheng and Siauw Ng
Catalysts 2019, 9(8), 689; https://doi.org/10.3390/catal9080689 - 15 Aug 2019
Cited by 13 | Viewed by 4517
Abstract
Waste cooking oil (WCO) hydrotreating to produce green diesel is good for both the environmental protection and energy recovery problems. The roles of catalyst support and reaction temperature on reactions during WCO hydrotreating process were evaluated over an unsupported and a commercial sulfided [...] Read more.
Waste cooking oil (WCO) hydrotreating to produce green diesel is good for both the environmental protection and energy recovery problems. The roles of catalyst support and reaction temperature on reactions during WCO hydrotreating process were evaluated over an unsupported and a commercial sulfided cobalt and molybdenum (CoMoS) catalyst supported by a mixture of Al2O3, TiO2, and SiO2. The presence of catalyst support helped to improve the dispersion and enlarge the surface area of CoMoS, and was found to be a key factor in reducing reaction temperature, in enhancing the hydrodeoxygenation (HDO) and hydrogenation capabilities, and in decreasing polymerization capability. The increase of reaction temperature strongly improved the deoxygenation, hydrogenation, and cracking reaction activities. Compared to the unsupported CoMoS, the supported one exhibited good deoxygenation and hydrogenation capabilities at 340 °C in WCO hydrotreating to produce diesel fraction; however, high temperature operation needs to be carefully controlled because it may cause overcracking and dehydrogenation. Full article
(This article belongs to the Special Issue Catalysis for the Production of Sustainable Fuels and Chemicals)
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13 pages, 4429 KiB  
Article
Application of Microwave in Hydrogen Production from Methane Dry Reforming: Comparison Between the Conventional and Microwave-Assisted Catalytic Reforming on Improving the Energy Efficiency
by Seyyedmajid Sharifvaghefi, Babak Shirani, Mladen Eic and Ying Zheng
Catalysts 2019, 9(7), 618; https://doi.org/10.3390/catal9070618 - 20 Jul 2019
Cited by 21 | Viewed by 4723
Abstract
The microwave-assisted dry reforming of methane over Ni and Ni–MgO catalysts supported on activated carbon (AC) was studied with respect to reducing reaction energy consumption. In order to optimize the reforming reaction using the microwave setup, an inclusive study was performed on the [...] Read more.
The microwave-assisted dry reforming of methane over Ni and Ni–MgO catalysts supported on activated carbon (AC) was studied with respect to reducing reaction energy consumption. In order to optimize the reforming reaction using the microwave setup, an inclusive study was performed on the effect of operating parameters, including the type of catalysts’ active metal and their concentration in the AC support, feed flow rate, and reaction temperature on the reaction conversion and H2/CO selectivity. The methane dry reforming was also carried out using conventional heating and the results were compared to those of microwave heating. The catalysts’ activity was increased under microwave heating and as a result, the feed conversion and hydrogen selectivity were enhanced in comparison to the conventional heating method. In addition, to improve the reactants’ conversion and products’ selectivity, the thermal analysis also clarified the crucial importance of microwave heating in enhancing the energy efficiency of the reaction compared to the conventional heating. Full article
(This article belongs to the Special Issue Catalysis for the Production of Sustainable Fuels and Chemicals)
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10 pages, 2171 KiB  
Communication
Enhancement of Light Olefins Selectivity Over N-Doped Fischer-Tropsch Synthesis Catalyst Supported on Activated Carbon Pretreated with KMnO4
by Zhipeng Tian, Chenguang Wang, Zhan Si, Chengyan Wen, Ying Xu, Wei Lv, Lungang Chen, Xinghua Zhang and Longlong Ma
Catalysts 2019, 9(6), 505; https://doi.org/10.3390/catal9060505 - 31 May 2019
Cited by 6 | Viewed by 3343
Abstract
Ammonium iron citrate was used as an iron precursor in order to prepare N-doped catalysts supported on KMnO4 pretreated activated carbon (10MnK-AC). Iron nitride was synthesized in company with the formation of α-Fe2O3 on 10MnK-AC. The characterizations of the [...] Read more.
Ammonium iron citrate was used as an iron precursor in order to prepare N-doped catalysts supported on KMnO4 pretreated activated carbon (10MnK-AC). Iron nitride was synthesized in company with the formation of α-Fe2O3 on 10MnK-AC. The characterizations of the catalysts show that nitrogen atoms were doped into iron lattice rather than the networks of the carbon support. The performance of Fischer-Tropsch synthesis to light olefins (FTO) suggest an improvement in O/P ratio (olefins to paraffins molar ratio of C2–C4) over the iron catalysts supported on 10MnK-AC. The further promotion of light olefins selectivity (up to 44.7%) was obtained over FeN-10MnK-AC catalyst owing to the collaborative contribution of the electron donor effect of nitrogen and the suppression effect on the second hydrogenation over 10MnK-AC support. Full article
(This article belongs to the Special Issue Catalysis for the Production of Sustainable Fuels and Chemicals)
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13 pages, 1640 KiB  
Article
Influence of Chemical Surface Characteristics of Ammonium-Modified Chilean Zeolite on Oak Catalytic Pyrolysis
by Serguei Alejandro-Martín, Adán Montecinos Acaricia, Cristian Cerda-Barrera and Hatier Díaz Pérez
Catalysts 2019, 9(5), 465; https://doi.org/10.3390/catal9050465 - 21 May 2019
Cited by 4 | Viewed by 3045
Abstract
The influence of chemical surface characteristics of Chilean natural and modified zeolites on Chilean Oak catalytic pyrolysis was investigated in this study. Chilean zeolite samples were characterised by nitrogen absorption at 77 K, X-ray powder diffraction (XRD), and X-ray fluorescence (XRF). The nature [...] Read more.
The influence of chemical surface characteristics of Chilean natural and modified zeolites on Chilean Oak catalytic pyrolysis was investigated in this study. Chilean zeolite samples were characterised by nitrogen absorption at 77 K, X-ray powder diffraction (XRD), and X-ray fluorescence (XRF). The nature and strength of zeolite acid sites were studied by diffuse reflectance infrared Fourier transform (DRIFT), using pyridine as a probe molecule. Experimental pyrolysis was conducted in a quartz cylindrical reactor and bio-oils were obtained by condensation of vapours in a closed container. Chemical species in bio-oil samples were identified by a gas chromatography/mass spectrophotometry (GC/MS) analytical procedure. Results indicate that after the ionic exchange treatment, an increase of the Brønsted acid site density and strength was observed in ammonium-modified zeolites. Brønsted acids sites were associated with an increment of the composition of ketones, aldehydes, and hydrocarbons and to a decrease in the composition of the following families (esters; ethers; and acids) in obtained bio-oil samples. The Brønsted acid sites on ammonium-modified zeolite samples are responsible for the upgraded bio-oil and value-added chemicals, obtained in this research. Bio-oil chemical composition was modified when the pyrolysis-derived compounds were upgraded over a 2NHZ zeolite sample, leading to a lower quantity of oxygenated compounds and a higher composition of value-added chemicals. Full article
(This article belongs to the Special Issue Catalysis for the Production of Sustainable Fuels and Chemicals)
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22 pages, 4339 KiB  
Article
The Promoting Effect of Ni on Glycerol Hydrogenolysis to 1,2-Propanediol with In Situ Hydrogen from Methanol Steam Reforming Using a Cu/ZnO/Al2O3 Catalyst
by Yuanqing Liu, Xiaoming Guo, Garry L. Rempel and Flora T. T. Ng
Catalysts 2019, 9(5), 412; https://doi.org/10.3390/catal9050412 - 01 May 2019
Cited by 19 | Viewed by 4310
Abstract
Production of green chemicals using a biomass derived feedstock is of current interest. Among the processes, the hydrogenolysis of glycerol to 1,2-propanediol (1,2-PD) using externally supplied molecular hydrogen has been studied quite extensively. The utilization of methanol present in crude glycerol from biodiesel [...] Read more.
Production of green chemicals using a biomass derived feedstock is of current interest. Among the processes, the hydrogenolysis of glycerol to 1,2-propanediol (1,2-PD) using externally supplied molecular hydrogen has been studied quite extensively. The utilization of methanol present in crude glycerol from biodiesel production can avoid the additional cost for molecular hydrogen storage and transportation, as well as reduce the safety risks due to the high hydrogen pressure operation. Recently the hydrogenolysis of glycerol with a Cu/ZnO/Al2O3 catalyst using in situ hydrogen generated from methanol steam reforming in a liquid phase reaction has been reported. This paper focusses on the effect of added Ni on the activity of a Cu/ZnO/Al2O3 catalyst prepared by an oxalate gel-co-precipitation method for the hydrogenolysis of glycerol using methanol as a hydrogen source. It is found that Ni reduces the conversion of glycerol but improves the selectivity to 1,2-PD, while a higher conversion of methanol is observed. The promoting effect of Ni on the selectivity to 1,2-PD is attributed to the slower dehydration of glycerol to acetol coupled with a higher availability of in situ hydrogen produced from methanol steam reforming and the higher hydrogenation activity of Ni towards the intermediate acetol to produce 1,2-PD. Full article
(This article belongs to the Special Issue Catalysis for the Production of Sustainable Fuels and Chemicals)
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16 pages, 3597 KiB  
Article
Hydrotreated Vegetable Oil as a Fuel from Waste Materials
by Petr Zeman, Vladimír Hönig, Martin Kotek, Jan Táborský, Michal Obergruber, Jakub Mařík, Veronika Hartová and Martin Pechout
Catalysts 2019, 9(4), 337; https://doi.org/10.3390/catal9040337 - 04 Apr 2019
Cited by 18 | Viewed by 14479
Abstract
Biofuels have become an integral part of everyday life in modern society. Bioethanol and fatty acid methyl esters are a common part of both the production of gasoline and diesel fuels. Also, pressure on replacing fossil fuels with bio-components is constantly growing. Waste [...] Read more.
Biofuels have become an integral part of everyday life in modern society. Bioethanol and fatty acid methyl esters are a common part of both the production of gasoline and diesel fuels. Also, pressure on replacing fossil fuels with bio-components is constantly growing. Waste vegetable fats can replace biodiesel. Hydrotreated vegetable oil (HVO) seems to be a better alternative. This fuel has a higher oxidation stability for storage purposes, a lower temperature of loss of filterability for the winter time, a lower boiling point for cold starts, and more. Viscosity, density, cold filter plugging point of fuel blend, and flash point have been measured to confirm that a fuel from HVO is so close to a fuel standard that it is possible to use it in engines without modification. The objective of this article is to show the properties of different fuels with and without HVO admixtures and to prove the suitability of using HVO compared to FAME. HVO can also be prepared from waste materials, and no major modifications of existing refinery facilities are required. No technology in either investment or engine adaptation of fuel oils is needed in fuel processing. Full article
(This article belongs to the Special Issue Catalysis for the Production of Sustainable Fuels and Chemicals)
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19 pages, 4848 KiB  
Article
Hydrotreatment Followed by Oxidative Desulfurization and Denitrogenation to Attain Low Sulphur and Nitrogen Bitumen Derived Gas Oils
by Sandeep Badoga, Prachee Misra, Girish Kamath, Ying Zheng and Ajay K. Dalai
Catalysts 2018, 8(12), 645; https://doi.org/10.3390/catal8120645 - 10 Dec 2018
Cited by 10 | Viewed by 5632
Abstract
To lower the sulphur content below 500 ppm and to increase the quality of bitumen derived heavy oil, a combination of hydrotreating followed by oxidative desulfurization (ODS) and oxidative denitrogenation (ODN) is proposed in this work. NiMo/γ-Al2O3 catalyst was synthesized [...] Read more.
To lower the sulphur content below 500 ppm and to increase the quality of bitumen derived heavy oil, a combination of hydrotreating followed by oxidative desulfurization (ODS) and oxidative denitrogenation (ODN) is proposed in this work. NiMo/γ-Al2O3 catalyst was synthesized and used to hydrotreat heavy gas oil (HGO) and light gas oil (LGO) at typical operating conditions of 370–390 °C, 9 MPa, 1–1.5 h−1 space velocity and 600:1 H2 to oil ratio. γ-Alumina and alumina-titania supported Mo, P, Mn and W catalysts were synthesized and characterized using X-ray diffractions, N2 adsorption-desorption using Brunauer–Emmett–Teller (BET) method, X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopy (FT-IR). All catalysts were tested for the oxidation of sulphur and nitrogen aromatic compounds present in LGO and HGO using tert-butyl hydroperoxide (TBHP) as oxidant. The oxidized sulphur and nitrogen compounds were extracted using adsorption on activated carbon and liquid-liquid extraction using methanol. The determination of oxidation states of each metal using XPS confirmed the structure of metal oxides in the catalyst. Thus, the catalytic activity determined in terms of sulphur and nitrogen removal is related to their physico-chemical properties. In agreement with literature, a simplistic mechanism for the oxidative desulfurization is also presented. Mo was found to be more active in comparison to W. Presence of Ti in the support has shown 8–12% increase in ODS and ODN. The MnPMo/γ-Al2O3-TiO2 catalyst showed the best activity for sulphur and nitrogen removal. The role of Mn and P as promoters to molybdenum was also discussed. Further three-stage ODS and ODN was performed to achieve less than 500 ppm in HGO and LGO. The combination of hydrotreatment, ODS and ODN has resulted in removal of 98.8 wt.% sulphur and 94.7 wt.% nitrogen from HGO and removal of 98.5 wt.% sulphur and 97.8 wt.% nitrogen from LGO. Full article
(This article belongs to the Special Issue Catalysis for the Production of Sustainable Fuels and Chemicals)
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18 pages, 4317 KiB  
Article
Influence of Bio-Oil Phospholipid on the Hydrodeoxygenation Activity of NiMoS/Al2O3 Catalyst
by Muhammad Abdus Salam, Derek Creaser, Prakhar Arora, Stefanie Tamm, Eva Lind Grennfelt and Louise Olsson
Catalysts 2018, 8(10), 418; https://doi.org/10.3390/catal8100418 - 25 Sep 2018
Cited by 16 | Viewed by 4033
Abstract
Hydrodeoxygenation (HDO) activity of a typical hydrotreating catalyst, sulfided NiMo/γ-Al2O3 for deoxygenation of a fatty acid has been explored in a batch reactor at 54 bar and 320 °C in the presence of contaminants, like phospholipids, which are known to [...] Read more.
Hydrodeoxygenation (HDO) activity of a typical hydrotreating catalyst, sulfided NiMo/γ-Al2O3 for deoxygenation of a fatty acid has been explored in a batch reactor at 54 bar and 320 °C in the presence of contaminants, like phospholipids, which are known to be present in renewable feeds. Oleic acid was used for the investigation. Freshly sulfided catalyst showed a high degree of deoxygenation activity; products were predominantly composed of alkanes (C17 and C18). Experiments with a major phospholipid showed that activity for C17 was greatly reduced while activity to C18 was not altered significantly in the studied conditions. Characterization of the spent catalyst revealed the formation of aluminum phosphate (AlPO4), which affects the active phase dispersion, blocks the active sites, and causes pore blockage. In addition, choline, formed from the decomposition of phospholipid, partially contributes to the observed deactivation. Furthermore, a direct correlation was observed in the accumulation of coke on the catalyst and the amount of phospholipid introduced in the feed. We therefore propose that the reason for the increased deactivation is due to the dual effects of an irreversible change in phase to aluminum phosphate and the formation of choline. Full article
(This article belongs to the Special Issue Catalysis for the Production of Sustainable Fuels and Chemicals)
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