Special Issue "Commemorative Issue in Honor of Professor Emeritus Calvin H. Bartholomew in Anticipation of His 75th Birthday"

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

Deadline for manuscript submissions: 31 December 2017

Special Issue Editor

Guest Editor
Assoc. Prof. Morris D. Argyle

Chemical Engineering Department, Brigham Young University, Provo, UT 84602, USA
Website | E-Mail
Phone: 801-422-6239
Interests: heterogeneous catalysis, energy engineering, plasma reactions, CO2 capture

Special Issue Information

Dear Colleagues,

Our journal is pleased to publish a commemorative issue in honor of Professor Emeritus Calvin H. Bartholomew in anticipation of his 75th birthday.
Calvin H. Bartholomew is the Professor Emeritus of Chemical Engineering at Brigham Young University (BYU). He received his BES degree from BYU and his PhD at Stanford University, where his advisor was Michel Boudart. Professor Bartholomew has taught and mentored students at BYU in catalysis, materials, and catalyst deactivation for 42 years. He is an active researcher in heterogeneous catalysis and a recognized authority on Fischer-Tropsch and catalyst deactivation; he has co-authored over 140 journal articles, 20 chapters/reviews, 6 books, and 6 patents. His works have received in excess of 7200 citations and their h-factor is 43. He is co-author, with Dr. Robert Farrauto, of Engelhard of Fundamentals of Industrial Catalytic Processes, a leading handbook and textbook. He has developed and taught short courses on “Heterogeneous Catalysis”, “Fischer Tropsch Synthesis”, and “Catalyst Deactivation” to more than 750 professionals from industry and academe. He has worked at Corning Inc., UnoCal, and Sandia National Labs and consulted with more than 75 company clients. He has consulted with a dozen plus start-up GTL companies and has been the principal motivator for the development of advanced supports and Fischer-Tropsch catalysts at Cosmas Inc.
In honor and recognition of Professor Bartholomew’s outstanding career contributions to the field of heterogeneous catalysis and in anticipation of his 75th birthday in 2018, this commemorative issue of Catalysts welcomes the submission of previously unpublished manuscripts from original work or reviews in the field of catalysis. We plan to receive submissions from 1 October 2016 to 31 December 2017 and manuscripts will be published online on an ongoing basis after being processed.

Assoc. Prof. Morris D. Argyle
Guest Editor

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Published Papers (6 papers)

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Research

Open AccessArticle Chiral Catalyst Deactivation during the Asymmetric Hydrogenation of Acetophenone
Catalysts 2017, 7(7), 193; doi:10.3390/catal7070193
Received: 18 May 2017 / Revised: 14 June 2017 / Accepted: 20 June 2017 / Published: 23 June 2017
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Abstract
Asymmetric hydrogenation in solution catalyzed by chiral catalysts is a powerful tool to obtain chiral secondary alcohols. It is possible to reach conversions and enantiomeric excesses close to 99%, but that frequently requires the use of non-optimal amounts of catalysts or long reaction
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Asymmetric hydrogenation in solution catalyzed by chiral catalysts is a powerful tool to obtain chiral secondary alcohols. It is possible to reach conversions and enantiomeric excesses close to 99%, but that frequently requires the use of non-optimal amounts of catalysts or long reaction times. That is in part caused by the lack of kinetic information needed for the design of large-scale reactors, including few reported details about catalyst deactivation. In this work, we present a kinetic model for the asymmetric hydrogenation in solution of acetophenone, a prochiral substrate, catalyzed by different bisphosphine-diamine Ru complexes. The experimental data was fitted with a first order model that includes first order deactivation of the catalyst and the presence of residual activity. The fit of the experimental data is very good, and an analysis of the kinetic and deactivation parameters gives further insight into the role of each ligand present in the Ru catalysts. This is the first report of a kinetic analysis of homogenous complexes’ catalysis including an analysis of their deactivation. Full article
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Open AccessArticle Carbon-Modified Mesoporous Anatase/TiO2(B) Whisker for Enhanced Activity in Direct Synthesis of Hydrogen Peroxide by Palladium
Catalysts 2017, 7(6), 175; doi:10.3390/catal7060175
Received: 16 March 2017 / Revised: 17 May 2017 / Accepted: 22 May 2017 / Published: 2 June 2017
Cited by 2 | PDF Full-text (4823 KB) | HTML Full-text | XML Full-text | Supplementary Files
Abstract
The regulation of the interaction between H2O2 and its catalysts is a promising route to achieve high productivity and selectivity towards H2O2. Herein, mesoporous anatase/TiO2(B) whisker (mb-TiO2) modified with heterogeneous carbon was
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The regulation of the interaction between H2O2 and its catalysts is a promising route to achieve high productivity and selectivity towards H2O2. Herein, mesoporous anatase/TiO2(B) whisker (mb-TiO2) modified with heterogeneous carbon was prepared as the support of Pd-based catalysts for the direct synthesis of H2O2. The morphology and structure of the catalyst were investigated by transmission electron microscopy, X-ray diffraction, Raman spectroscopy, Brunner-Emmet-Teller measurements, and X-ray photoelectron spectroscopy. The interaction between H2O2 and the support was studied by isothermal calorimeter. The carbon heterogeneous modification can weaken the interaction between H2O2 and the support, then accelerate the desorption of H2O2 and reduce the re-adsorption of H2O2 in the reaction medium. Meanwhile, the synergistic effects between TiO2 and Pd nanoparticles are not influenced by the heterogeneous carbon distribution. The catalyst exhibits better performance for the synthesis of H2O2 compared with the corresponding unmodified catalyst; the productivity of H2O2 increases more than 40%, which can be ascribed to the decrease of further H2O2 conversion under the weakened interaction. Full article
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Open AccessFeature PaperArticle Development of Active and Stable Low Nickel Content Catalysts for Dry Reforming of Methane
Catalysts 2017, 7(5), 157; doi:10.3390/catal7050157
Received: 30 March 2017 / Revised: 11 May 2017 / Accepted: 12 May 2017 / Published: 16 May 2017
Cited by 2 | PDF Full-text (6003 KB) | HTML Full-text | XML Full-text
Abstract
Methane dry reforming (DRM) was investigated over highly active Ni catalysts with low metal content (2.5 wt %) supported on Mg-Al mixed oxide. The aim was to minimize carbon deposition and metal sites agglomeration on the working catalyst which are known to cause
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Methane dry reforming (DRM) was investigated over highly active Ni catalysts with low metal content (2.5 wt %) supported on Mg-Al mixed oxide. The aim was to minimize carbon deposition and metal sites agglomeration on the working catalyst which are known to cause catalyst deactivation. The solids were characterized using N2 adsorption, X-ray diffraction, temperature-programmed reduction, X-ray photoelectron spectroscopy, and UV-Vis diffuse reflectance spectroscopy. The results showed that MgO-Al2O3 solid solution phases are obtained when calcining Mg-Al hydrotalcite precursor in the temperature range of 550–800 °C. Such phases contribute to the high activity of catalysts with low Ni content even at low temperature (500 °C). Modifying the catalyst preparation with citric acid significantly slows the coking rate and reduces the size of large octahedrally coordinated NiO-like domains, which may easily agglomerate on the surface during DRM. The most effective Ni catalyst shows a stable DRM course over 60 h at high weight hourly space velocity with very low coke deposition. This is a promising result for considering such catalyst systems for further development of an industrial DRM technology. Full article
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Open AccessArticle Methanation of CO2 on Ni/Al2O3 in a Structured Fixed-Bed Reactor—A Scale-Up Study
Catalysts 2017, 7(5), 152; doi:10.3390/catal7050152
Received: 31 March 2017 / Revised: 24 April 2017 / Accepted: 4 May 2017 / Published: 15 May 2017
Cited by 1 | PDF Full-text (9418 KB) | HTML Full-text | XML Full-text
Abstract
Due to the ongoing change of energy supply, the availability of a reliable high-capacity storage technology becomes increasingly important. While conventional large-scale facilities are either limited in capacity respective supply time or their extension potential is little (e.g., pumped storage power stations), decentralized
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Due to the ongoing change of energy supply, the availability of a reliable high-capacity storage technology becomes increasingly important. While conventional large-scale facilities are either limited in capacity respective supply time or their extension potential is little (e.g., pumped storage power stations), decentralized units could contribute to energy transition. The concepts of PtX (power-to-X) storage technologies and in particular PtG (power-to-gas) aim at fixation of electric power in chemical compounds. CO2 hydrogenation (methanation) is the foundation of the PtG idea as H2 (via electrolysis) and CO2 are easily accessible. Methane produced in this way, often called substitute natural gas (SNG), is a promising solution since it can be stored in the existing gas grid, tanks or underground cavern storages. Methanation is characterized by a strong exothermic heat of reaction which has to be handled safely. This work aims at getting rid of extreme temperature hot-spots in a tube reactor by configuring the catalyst bed structure. Proof of concept studies began with a small tube reactor (V = 12.5 cm3) with a commercial 18 wt % Ni/Al2O3 catalyst. Later, a double-jacket tube reactor was built (V = 452 cm3), reaching a production rate of 50 L/h SNG. The proposed approach not only improves the heat management and process safety, but also increases the specific productivity and stability of the catalyst remarkably. Full article
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Open AccessFeature PaperArticle Methanol Steam Reforming: Na Doping of Pt/YSZ Provides Fine Tuning of Selectivity
Catalysts 2017, 7(5), 148; doi:10.3390/catal7050148
Received: 14 March 2017 / Revised: 10 April 2017 / Accepted: 3 May 2017 / Published: 10 May 2017
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Abstract
In this work, we found that sodium doping can be used to improve CO2 selectivity for supported Pt catalyst during methanol steam reforming. These materials are usually very active in the low temperature range; however, they are characterized by high selectivity of
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In this work, we found that sodium doping can be used to improve CO2 selectivity for supported Pt catalyst during methanol steam reforming. These materials are usually very active in the low temperature range; however, they are characterized by high selectivity of CO, which is a poison in downstream polymer electrolyte membrane fuel cells (PEM-FC) application. With Na doping, we found that CO2 selectivity was higher than 90% when 2.5 wt.% of sodium was added to Pt/YSZ. We have speculated that the different product distribution is due to a different reaction pathway being opened for CH3OH decomposition. Methanol decarbonylation was favored when Na was absent or low, while a formate decarboxylation pathway was favored when Na content reached 2.5 wt.%. The proposal is rooted in the observed weakening of the C-H bond of formate, as demonstrated in in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and kinetic isotope effect (KIE) experiments for the water-gas shift reaction conducted at low temperature. When adsorbed methoxy, produced when methanol is dissociatively adsorbed, was converted in the presence of H2O in DRIFTS spectroscopy, formate species were prevalent for a 2% Pt–2.5% Na/YSZ catalyst, while only a minor contribution was observed for 2% Pt/YSZ. Moreover, the formate produced on Na-doped Pt/YSZ exhibited ν(CH) stretching bands at low wavenumber, consistent with C–H bond weakening, thus favoring dehydrogenation (and decarboxylation). It is proposed that when Na is present, formate is likely an intermediate, and because its dehydrogenation is favored, selectivity can be fine-tuned between decarbonylation and decarboxylation based on Na dopant level. Full article
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Open AccessArticle Catalysts Promoted with Niobium Oxide for Air Pollution Abatement
Catalysts 2017, 7(5), 144; doi:10.3390/catal7050144
Received: 31 March 2017 / Revised: 1 May 2017 / Accepted: 4 May 2017 / Published: 8 May 2017
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Abstract
Pt-containing catalysts are currently used commercially to catalyze the conversion of carbon monoxide (CO) and hydrocarbon (HC) pollutants from stationary chemical and petroleum plants. It is well known that Pt-containing catalysts are expensive and have limited availability. The goal of this research is
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Pt-containing catalysts are currently used commercially to catalyze the conversion of carbon monoxide (CO) and hydrocarbon (HC) pollutants from stationary chemical and petroleum plants. It is well known that Pt-containing catalysts are expensive and have limited availability. The goal of this research is to find alternative and less expensive catalysts to replace Pt for these applications. This study found that niobium oxide (Nb2O5), as a carrier or support for certain transition metal oxides, promotes oxidation activity while maintaining stability, making them candidates as alternatives to Pt. The present work reports that the orthorhombic structure of niobium oxide (formed at 800 °C in air) promotes Co3O4 toward the oxidation of both CO and propane, which are common pollutants in volatile organic compound (VOC) applications. This was a surprising result since this structure of Nb2O5 has a very low surface area (about 2 m2/g) relative to the more traditional Al2O3 support, with a surface area of 150 m2/g. The results reported demonstrate that 1% Co3O4/Nb2O5 has comparable fresh and aged catalytic activity to 1% Pt/γ-Al2O3 and 1% Pt/Nb2O5. Furthermore, 6% Co3O4/Nb2O5 outperforms 1% Pt/Al2O3 in both catalytic activity and thermal stability. These results suggest a strong interaction between niobium oxide and the active component—cobalt oxide—likely by inducing an oxygen defect structure with oxygen vacancies leading to enhanced activity toward the oxidation of CO and propane. Full article
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