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

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

Deadline for manuscript submissions: closed (31 December 2017) | Viewed by 60165

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Dr. Morris D. Argyle

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Chemical Engineering Department, Brigham Young University, Provo, UT 84602, USA
Interests: heterogeneous catalysis; energy engineering; plasma reactions; coal gasification; carbon dioxide capture and storage
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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anticipation of his 75th birthday in 2018, this commemorative issue of Catalysts welcomes the submission of previously unpublished manuscripts from original work or reviews in the field of catalysis.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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Advances in Catalyst Deactivation in Catalysts (9 articles)

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Editorial

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4 pages, 769 KiB

Open AccessEditorial

Commemorative Issue in Honor of Professor Calvin H. Bartholomew’s 75th Birthday

by Morris D. Argyle

Catalysts 2018, 8(11), 533; https://doi.org/10.3390/catal8110533 - 9 Nov 2018

Viewed by 2539

Abstract

This editorial is written to recognize Professor Emeritus Calvin H. Bartholomew, who celebrated his 75th birthday in 2018, and to introduce the commemorative issue of Catalysts compiled in his honor. Following a brief biography that celebrates the career and contributions of Professor Bartholomew, the nine articles that make up the special issue are briefly reviewed. Dr. Bartholomew is an eminent researcher, an outstanding educator, mentor, and friend. Full article

(This article belongs to the Special Issue Commemorative Issue in Honor of Professor Emeritus Calvin H. Bartholomew in Anticipation of His 75th Birthday)

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Research

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17 pages, 3581 KiB

Open AccessArticle

Effect of Support Pretreatment Temperature on the Performance of an Iron Fischer–Tropsch Catalyst Supported on Silica-Stabilized Alumina

by Kamyar Keyvanloo, Baiyu Huang, Trent Okeson, Hussein H. Hamdeh and William C. Hecker

Catalysts 2018, 8(2), 77; https://doi.org/10.3390/catal8020077 - 12 Feb 2018

Cited by 18 | Viewed by 4956

Abstract

The effect of support material pretreatment temperature, prior to adding the active phase and promoters, on Fischer–Tropsch activity and selectivity was explored. Four iron catalysts were prepared on silica-stabilized alumina (AlSi) supports pretreated at 700 °C, 900 °C, 1100 °C or 1200 °C. Addition of 5% silica to alumina made the AlSi material hydrothermally stable, which enabled the unusually high support pretreatment temperatures (>900 °C) to be studied. High-temperature dehydroxylation of the AlSi before impregnation greatly reduces FeO·Al₂O₃ surface spinel formation by removing most of the support-surface hydroxyl groups leading to more effectively carbided catalyst. The activity increases more than four-fold for the support calcined at elevated temperatures (1100–1200 °C) compared with traditional support calcination temperatures of <900 °C. This unique pretreatment also facilitates the formation of ε′-Fe_2.2C rather than χ-Fe_2.5C on the AlSi support, which shows an excellent correlation with catalyst productivity. Full article

(This article belongs to the Special Issue Commemorative Issue in Honor of Professor Emeritus Calvin H. Bartholomew in Anticipation of His 75th Birthday)

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20 pages, 6047 KiB

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In Situ UV-Visible Assessment of Iron-Based High-Temperature Water-Gas Shift Catalysts Promoted with Lanthana: An Extent of Reduction Study

by Basseem B. Hallac, Jared C. Brown, Eli Stavitski, Roger G. Harrison and Morris D. Argyle

Catalysts 2018, 8(2), 63; https://doi.org/10.3390/catal8020063 - 4 Feb 2018

Cited by 8 | Viewed by 5067

Abstract

The extent of reduction of unsupported iron-based high-temperature water-gas shift catalysts with small (<5 wt %) lanthana contents was studied using UV-visible spectroscopy. Temperature- programmed reduction measurements showed that lanthana content higher than 0.5 wt % increased the extent of reduction to metallic Fe, while 0.5 wt % of lanthana facilitated the reduction to Fe₃O₄. In situ measurements on the iron oxide catalysts using mass and UV-visible spectroscopies permitted the quantification of the extent of reduction under temperature-programmed reduction and high-temperature water-gas shift conditions. The oxidation states were successfully calibrated against normalized absorbance spectra of visible light using the Kubelka-Munk theory. The normalized absorbance relative to the fully oxidized Fe₂O₃ increased as the extent of reduction increased. XANES suggested that the average bulk iron oxidation state during the water-gas shift reaction was Fe^+2.57 for the catalyst with no lanthana and Fe^+2.54 for the catalysts with 1 wt % lanthana. However, the UV-vis spectra suggest that the surface oxidation state of iron would be Fe^+2.31 for the catalyst with 1 wt % lanthana if the oxidation state of iron in the catalyst with 0 wt % lanthana were Fe^+2.57. The findings of this paper emphasize the importance of surface sensitive UV-visible spectroscopy for determining the extent of catalyst reduction during operation. The paper highlights the potential to use bench-scale UV-visible spectroscopy to study the surface chemistry of catalysts instead of less-available synchrotron X-ray radiation facilities. Full article

(This article belongs to the Special Issue Commemorative Issue in Honor of Professor Emeritus Calvin H. Bartholomew in Anticipation of His 75th Birthday)

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13 pages, 3904 KiB

Open AccessArticle

Structural Changes of Highly Active Pd/MeO_x (Me = Fe, Co, Ni) during Catalytic Methane Combustion

by Dominik Seeburg, Dongjing Liu, Joerg Radnik, Hanan Atia, Marga-Martina Pohl, Matthias Schneider, Andreas Martin and Sebastian Wohlrab

Catalysts 2018, 8(2), 42; https://doi.org/10.3390/catal8020042 - 23 Jan 2018

Cited by 19 | Viewed by 4924

Abstract

Fe₂O₃, Co₃O₄ and NiO nanoparticles were prepared via a citrate method and further functionalized with Pd by impregnation. The pure oxides as well as Pd/Fe₂O₃, Pd/Co₃O₄, and Pd/NiO (1, 5 and 10 wt % Pd) were employed for catalytic methane combustion under methane lean (1 vol %)/oxygen rich (18 vol %, balanced with nitrogen) conditions. Already, the pure metal oxides showed a high catalytic activity leading to complete conversion temperature of T₁₀₀ ≤ 500 °C. H₂-TPR (Temperature-programmed reduction) experiments revealed that Pd-functionalized metal oxides exhibited enhanced redox activity compared to the pure oxides leading to improved catalytic combustion activity at lower temperatures. At a loading of 1 wt % Pd, 1Pd/Co₃O₄ (T₁₀₀ = 360 °C) outperforms 1Pd/Fe₂O₃ (T₁₀₀ = 410 °C) as well as 1Pd/NiO (T₁₀₀ = 380 °C). At a loading of 10 wt % Pd, T₁₀₀ could only be slightly reduced in all cases. 1Pd/Co₃O₄ and 1Pd/NiO show reasonable stability over 70 h on stream at T₁₀₀. XPS (X-ray photoelectron spectroscopy) and STEM (Scanning transmission electron microscopy) investigations revealed strong interactions between Pd and NiO as well as Co₃O₄, respectively, leading to dynamic transformations and reoxidation of Pd due to solid state reactions, which leads to the high long-term stability. Full article

(This article belongs to the Special Issue Commemorative Issue in Honor of Professor Emeritus Calvin H. Bartholomew in Anticipation of His 75th Birthday)

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1445 KiB

Open AccessArticle

Chiral Catalyst Deactivation during the Asymmetric Hydrogenation of Acetophenone

by Jose P. Ruelas-Leyva and Gustavo A. Fuentes

Catalysts 2017, 7(7), 193; https://doi.org/10.3390/catal7070193 - 23 Jun 2017

Cited by 6 | Viewed by 5422

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 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

(This article belongs to the Special Issue Commemorative Issue in Honor of Professor Emeritus Calvin H. Bartholomew in Anticipation of His 75th Birthday)

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4823 KiB

Open AccessArticle

Carbon-Modified Mesoporous Anatase/TiO₂(B) Whisker for Enhanced Activity in Direct Synthesis of Hydrogen Peroxide by Palladium

by Rui Tu, Licheng Li, Suoying Zhang, Shuying Chen, Jun Li and Xiaohua Lu

Catalysts 2017, 7(6), 175; https://doi.org/10.3390/catal7060175 - 2 Jun 2017

Cited by 16 | Viewed by 5549

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 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

(This article belongs to the Special Issue Commemorative Issue in Honor of Professor Emeritus Calvin H. Bartholomew in Anticipation of His 75th Birthday)

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6003 KiB

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Development of Active and Stable Low Nickel Content Catalysts for Dry Reforming of Methane

by Quan Luu Manh Ha, Udo Armbruster, Hanan Atia, Matthias Schneider, Henrik Lund, Giovanni Agostini, Jörg Radnik, Huyen Thanh Vuong and Andreas Martin

Catalysts 2017, 7(5), 157; https://doi.org/10.3390/catal7050157 - 16 May 2017

Cited by 51 | Viewed by 7544

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 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

(This article belongs to the Special Issue Commemorative Issue in Honor of Professor Emeritus Calvin H. Bartholomew in Anticipation of His 75th Birthday)

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9418 KiB

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Methanation of CO₂ on Ni/Al₂O₃ in a Structured Fixed-Bed Reactor—A Scale-Up Study

by Daniel Türks, Hesham Mena, Udo Armbruster and Andreas Martin

Catalysts 2017, 7(5), 152; https://doi.org/10.3390/catal7050152 - 15 May 2017

Cited by 44 | Viewed by 11375

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 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

(This article belongs to the Special Issue Commemorative Issue in Honor of Professor Emeritus Calvin H. Bartholomew in Anticipation of His 75th Birthday)

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4667 KiB

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Methanol Steam Reforming: Na Doping of Pt/YSZ Provides Fine Tuning of Selectivity

by Michela Martinelli, Gary Jacobs, Uschi M. Graham and Burtron H. Davis

Catalysts 2017, 7(5), 148; https://doi.org/10.3390/catal7050148 - 10 May 2017

Cited by 15 | Viewed by 5949

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 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

(This article belongs to the Special Issue Commemorative Issue in Honor of Professor Emeritus Calvin H. Bartholomew in Anticipation of His 75th Birthday)

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2873 KiB

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Catalysts Promoted with Niobium Oxide for Air Pollution Abatement

by Wendi Xiang, Xiaochen Han, Jennifer Astorsdotter and Robert Farrauto

Catalysts 2017, 7(5), 144; https://doi.org/10.3390/catal7050144 - 8 May 2017

Cited by 5 | Viewed by 5260

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 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

(This article belongs to the Special Issue Commemorative Issue in Honor of Professor Emeritus Calvin H. Bartholomew in Anticipation of His 75th Birthday)

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