Article
Chemistry, Inorganic & Nuclear
Risheng Wang, Zhihua Peng, Pingping Wu, Hongman Sun, Yu Zhang, Fazle Subhan, Hailiang Yin, Youhe Wang, Zifeng Yan
Summary: This study presents a novel approach to synthesize nanorod stacked hierarchical ZSM-48 (NSH-ZSM-48) using a newly designed organic structure-directing agent (OSDA). The synthesized NSH-ZSM-48 exhibits abundant mesopores and high surface area, leading to enhanced catalytic activity and selectivity in the selective oxidation of cyclohexane.
INORGANIC CHEMISTRY FRONTIERS
(2022)
Article
Engineering, Chemical
Nebojsa Korica, Pedro S. F. Mendes, Jeriffa De Clercq, Joris W. Thybaut
Summary: The study found that the presence of methylcyclohexane affects the hydroconversion of n-octane over Pt/HUSY catalysts, but does not impact the behavior of methylcyclohexane itself. This is mainly due to the preferred adsorption of cycloalkanes on metal sites, leading to a shift from ideal to nonideal hydrocracking.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2021)
Review
Chemistry, Physical
Dmitry Yu. Murzin
Summary: This mini-review addresses the kinetic features of single-site catalysis, including both qualitative and quantitative aspects.
Article
Chemistry, Multidisciplinary
Xinyu Li, He Han, Wenqian Xu, Son-Jong Hwang, Zhichen Shi, Peng Lu, Aditya Bhan, Michael Tsapatsis
Summary: Low-silica faujasite zeolites sustain framework integrity and porosity upon moderate ion exchange, introducing two kinds of protons within supercages. Protons on site II exhibit higher reactivity for propane reactions compared to protons on site III. Low-silica proton-form FAU zeolites possess protons on site III and provide high-temperature structural and chemical stability, enabling their application as solid-acid catalysts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Umang Agarwal, Marcello S. Rigutto, Erik Zuidema, A. P. J. Jansen, Ali Poursaeidesfahani, Shrinjay Sharma, David Dubbeldam, Thijs J. H. Vlugt
Summary: A reactor model that deconvolutes the thermodynamics of hydrocarbon adsorption and intraporous reaction kinetics in zeolite Beta was studied using Configurational-bias Monte Carlo simulations. The model provides a quantitative description of significant reactions and determines the activation enthalpies of different reactions. The model can be used to investigate the effect of pore structure on adsorption and reaction kinetics.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Physical
Jan Droenner, Karim Bijerch, Peter Hausoul, Regina Palkovits, Matthias Eisenacher
Summary: Hydroxybenzene, also known as phenol, is a crucial organic commodity chemical, and the cumene process is widely used for its production. The Hock rearrangement is a vital step in this process, and the use of high-temperature-treated Linde Type X (LTX) zeolites as catalysts in the peroxide cleavage step showed promising results, making it a potential alternative to sulfuric acid for this reaction.
Article
Environmental Sciences
Cesar C. Martins, Michelle Alves de Abreu-Mota, Mylene Giseli do Nascimento, Ana Lucia L. Dauner, Rafael Andre Lourenco, Marcia C. Bicego, Rosalinda C. Montone
Summary: Organic biomarkers, such as aliphatic hydrocarbons, have been widely used to evaluate recent environmental changes in marine environments, including Antarctica. The sources of aliphatic hydrocarbons in Antarctic sediment cores have remained stable, with a slight increase in inputs observed between 1975 and 1992.
SCIENCE OF THE TOTAL ENVIRONMENT
(2021)
Article
Chemistry, Applied
Hao Qin, Nengjie Feng, Quan Lv, Hui Wan, Guofeng Guan
Summary: In this study, Pt single atoms were anchored on the catalyst surface using cerium oxide as a binder. Pt1@CeOx/SAPO-11 exhibited significant activity and effectively inhibited the selectivity of cracking or hydrogenolysis. The catalytic efficiency of this reaction can be improved by dispersing the active sites to reduce the local concentration of the product of a reversible step in an intermediate reaction.
FUEL PROCESSING TECHNOLOGY
(2023)
Article
Engineering, Chemical
Qiang Wang, Huici Shan, Ley Boon Sim, Jianrong Xie, Songshou Ye, Jile Fu, Jiexiang Wang, Nuowei Zhang, Jinbao Zheng, Binghui Chen
Summary: ZSM-22 zeolites were synthesized using different structure-directing agents (SDAs) with varying alkyl chain lengths, and the resulting samples showed varying morphology and acidity. Pt/ZSM-22 catalysts exhibited improved activity and selectivity in n-hexadecane hydroisomerization, with higher alkyl chain lengths of SDAs leading to higher yields.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Chemistry, Multidisciplinary
Fabian Berger, Joachim Sauer
Summary: Quantum chemical evidence demonstrates that dimerization of linear butenes and pentenes at zeolitic Bronsted sites in H-MFI results in the formation of alkanes featuring cyclohexane rings instead of branched alkenes. Calculations show close agreement between the calculated reaction enthalpies for cyclic alkanes and the experimental values, while branched alkoxide formation enthalpy deviates significantly from experiment. Additionally, calculated IR spectra reveal the observed conversion of the OH group, indicating changes in interactions with alkenes and alkanes.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Karam B. Idrees, Kent O. Kirlikovali, Caitlin Setter, Haomiao Xie, Helen Brand, Bhajan Lal, Fanrui Sha, Courtney S. Smoljan, Xiaoliang Wang, Timur Islamoglu, Lauren K. Macreadie, Omar K. Farha
Summary: Hexane isomers are important in the petrochemical industry but separating them poses challenges. Traditional thermal separation methods are energy-intensive, so there is a growing demand for less energy-intensive nonthermal methods. Adsorption-based methods using MOFs have emerged as promising alternatives. In this study, two novel MOFs, NU-2004 and NU-2005, were successfully synthesized and showed exceptional thermal stability and structural rigidity, making significant advancements in hexane isomer separation compared to other MOFs.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Pandong Ma, Yubing Li, Hexun Zhou, Mengheng Wang, Mengsi Zhu, Yaoyao Han, Xin Zhang, Kang Cheng, Abhishek Dutta Chowdhury
Summary: Redox-acid bifunctional zeolites have unique physicochemical properties that make them essential in the petrochemical industry, particularly in the hydro-conversion of linear alkanes to produce high-octane fuels. Current research focuses on evaluating the communication criteria between catalytically active sites and reducing the use of noble metals in catalysis. However, the chemistry behind the interaction mode between metallic and acid sites during the hydro-conversion of n-alkanes over Pt or Pd/zeolites remains largely unexplored.
MATERIALS TODAY CHEMISTRY
(2023)
Article
Chemistry, Physical
Kareem Yusuf, Anusree Natraj, Kelvin Li, Mohamed Ateia, Zeid A. ALOthman, William R. Dichtel
Summary: Two-dimensional polymers in the form of layered covalent organic frameworks (COFs) show promise as adsorbent-based separations due to their tunable properties. High-quality single crystals of two 2D COFs exhibit improved separation characteristics in gas chromatography compared to polycrystalline samples. In this study, inverse pulse gas chromatography was used to characterize the dispersive and specific adsorption properties of single-crystalline and polycrystalline COFs for the separation of linear n-alkanes and polar probes.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Lijun Lu, Feiyu Qiu, Hesham Alhumade, Heng Zhang, Aiwen Lei
Summary: This work demonstrated metal-controlled mono-and double-carbonylation reactions of alkanes with amines, resulting in the preparation of alkyl amides and alkyl alpha-ketoamides, with Co and Cu catalysis systems affording different selectivities.
Article
Energy & Fuels
Larissa Brito, Gerhard D. Pirngruber, Emanuelle Guillon, Florian Albrieux, Johan A. Martens
Summary: The study on hydroisomerization and hydrocracking of octylcyclohexane using a bifunctional Pt/USY zeolite catalyst reveals a kinetic competition between isomerization and cracking, leading to favorable cracking distribution upon molecule tribranching.
Article
Chemistry, Analytical
Hannah Vanderschaeghe, Maarten Houlleberghs, Loes Verheyden, Dirk Dom, C. Vinod Chandran, Sambhu Radhakrishnan, Johan A. Martens, Eric Breynaert
Summary: Porous silica is commonly used to enhance the bioavailability of poorly soluble compounds in drug delivery. Traditional methods for residual solvent quantification in drug formations are tedious and involve extraction and capillary gas chromatography. This study presents a new method using magic-angle spinning nuclear magnetic resonance spectroscopy, originally developed for water quantification in zeolites. The results show that the initial water content of the silica carrier can impact the residual solvent concentration in drug-loaded materials.
ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Physical
Larissa Brito, Francois Payan, Florian Albrieux, Emmanuelle Guillon, Johan A. Martens, Gerhard D. Pirngruber
Summary: This study investigated the hydroisomerization and hydrocracking of octylcyclohexane over Pt and NiMoS-supported catalysts. The experiments were conducted at 300 degrees C and 60 bar, with a molar H-2 to hydrocarbon ratio of 7:1. The bifunctional catalysts, with acid function represented by large-pore zeolites or amorphous silica-alumina, showed higher activity in isomerization and cracking reactions. The comparison of reactivity with other compounds was also discussed.
Editorial Material
Chemistry, Physical
Javier Perez-Ramirez, Bert M. Weckhuysen, Maria E. Southall
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Review
Chemistry, Multidisciplinary
Foster Lubbe, Jan Ronge, Tom Bosserez, Johan A. Martens
Summary: Hydrogen is classified and labeled based on the resources and processes used in its production, such as electrolysis, and energy sources, such as solar radiation. Green hydrogen is primarily produced through the electrolysis of water using renewable electricity from wind, geothermal, solar, or hydroelectric power plants. Solar hydrogen generators, which integrate sunlight harvesting and water molecule splitting, are more modular and operate at a smaller scale. The term "golden hydrogen" is proposed to differentiate hydrogen produced by modular solar hydrogen generators. Decentralized modular production of golden hydrogen complements centralized and energy-intensive green hydrogen production. The distinction between green hydrogen and golden hydrogen can help promote the additionality principle in clean hydrogen policies.
CURRENT OPINION IN GREEN AND SUSTAINABLE CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Dario Poier, Sharon Mitchell, Victor Tulus, Gonzalo Guillen-Gosalbez, Javier Perez-Ramirez, Roger Marti
Summary: Scaling up syntheses from mg to kg quantities is a complex endeavor, which requires adaptation to industrial processes, equipment, safety assessments, and environmental impact reduction. Transition metal single-atom heterogeneous catalysts (SAC), as a novel class of catalytic materials, could be a key approach to replace single-use catalysts and address the challenges in large-scale synthesis.
Article
Chemistry, Multidisciplinary
Sebastiano C. D'Angelo, Antonio J. Martin, Gonzalo Guillen-Gosalbez, Javier Perez-Ramirez
Summary: Intense efforts have been devoted to developing green and blue centralised Haber-Bosch processes, but a decentralised and sustainable scheme has yet to be assessed. In this study, we reveal the conditions under which small-scale systems based on the electrocatalytic reduction of nitrogen (eN2R) powered by photovoltaic energy (NH3-leaf) could become a competitive technology in terms of environmental criteria. The disclosed sustainability potential of NH3-leaf makes it a strong ally of gHB toward a non-fossil ammonia production.
Article
Chemistry, Physical
Hannelore Geerts-Claes, Sam Smet, Christoph Hengst, Frank-Walter Schuetze, Elke Verheyen, Matthias Minjauw, Christophe Detavernier, Sreeprasanth Pulinthanathu Sree, Johan Martens
Summary: This study investigates the mechanism of NOx adsorption on a Pd/FER zeolite in gas mixtures containing CO, O2, and H2O. It is found that oxidized palladium is required for achieving NOx adsorption, while clustered zerovalent palladium reduced with H2 cannot adsorb NOx in the presence of O2. The study provides evidence for a reaction mechanism involving oxygen-bridged PdII-O-PdII moieties of PdO nanoclusters, and the NO adsorption site on palladium is obtained by reducing one of the two PdII atoms to the zerovalent state, which is more readily achieved with CO compared to NO, explaining the beneficial role of CO.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Ewoud Vaneeckhaute, Jean-Max Tyburn, James G. Kempf, Johan A. Martens, Eric Breynaert
Summary: Amino acids and ammonia are essential metabolic markers for nitrogen metabolism and cellular regulation. This study demonstrates a high-field approach using NMR to investigate these metabolic pathways, providing a valuable alternative to existing techniques. By designing a specialized catalyst, spin order can be transferred from p-H-2 to N-15, allowing for reversible hyperpolarization of alanine and ammonia under ambient conditions. The stereochemistry and kinetics of these catalyst complexes are determined using isotopological fingerprinting and 2D-ZQ-NMR.
Article
Chemistry, Multidisciplinary
Thaylan Pinheiro Araujo, Jordi Morales-Vidal, Georgios Giannakakis, Cecilia Mondelli, Henrik Eliasson, Rolf Erni, Joseph A. Stewart, Sharon Mitchell, Nuria Lopez, Javier Perez-Ramirez
Summary: Ternary Pd-In2O3/ZrO2 catalysts prepared by wet impregnation exhibit selective and stable architecture under CO2 hydrogenation conditions, irrespective of the order of addition of Pd and In phases on the zirconia carrier. The rapid restructuring of the catalysts is driven by the metal-metal oxide interaction energetics. The presence of InPdx alloy particles decorated by InOx layers prevents performance losses associated with Pd sintering.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Lin Dong, Jordi Morales-Vidal, Lili Mu, Licheng Li, Nuria Lopez, Javier Perez-Ramirez, Zupeng Chen
Summary: In this study, an efficient selective synthesis of 5-Methylfurfural (MF) from 5-hydroxymethylfurfural (HMF) was achieved using an anatase-supported gold catalyst (Au/a-TiO2). The C-O bond was maintained during the hydrogenolysis of HMF, resulting in a high yield of 83.1% for MF. The superior performance of Au/a-TiO2 can be attributed to the high concentration of oxygen vacancies in the support, which limits H access, reduces reactant adsorption, and prevents condensation. This research highlights a new approach for the selective transformation of renewable compounds into high-value-added chemicals.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Biochemistry & Molecular Biology
Sambhu Radhakrishnan, Sam Smet, C. Vinod Chandran, Sreeprasanth Pulinthanathu Sree, Karel Duerinckx, Gina Vanbutsele, Johan A. Martens, Eric Breynaert
Summary: Selective catalytic reduction (SCR) is a major technology for reducing emissions from diesel engines, and variable temperature NMR can be used to predict the activity of Cu-zeolite SCR catalysts.
Article
Chemistry, Multidisciplinary
Phil Preikschas, Antonio J. J. Martin, Boon Siang Yeo, Javier Perez-Ramirez
Summary: Phosphate-derived nickel catalysts have been used to produce multicarbon products through CO2 electroreduction, but the effects of operating conditions on product formation are still unclear. In this study, refined H-1 NMR spectroscopy protocols were developed and combined with an automated NMR data processing routine to quantify carbon product formation under various parameters. The findings revealed performance trends in carbon product formation and identified four previously unreported compounds.
COMMUNICATIONS CHEMISTRY
(2023)
Article
Multidisciplinary Sciences
Emile Jules Beckwee, Geert Watson, Maarten Houlleberghs, Daniel Arenas Esteban, Sara Bals, Pascal Van Der Voort, Eric Breynaert, Johan Martens, Gino Baron, Joeri F. M. Denayer
Summary: This study reports a new type of periodic mesoporous organosilica (PMO) nanotubes, referred to as hollow ring PMO (HR-PMO), capable of promoting methane clathrate hydrate formation under mild working conditions and at high water loading. The HR-PMO nanotubes exhibit a steep single-stepped isotherm and a noticeably high methane storage capacity. Supported by ex situ cryo-electron tomography and x-ray diffraction, the findings suggest that HR-PMO nanotubes promote clathrate hydrate nucleation and growth by distributing and confining water in the mesopores of their outer wall, central channels, and external surface. These results highlight the potential application of organosilica materials for pressure-based storage of biomethane in confined clathrate hydrates.
Article
Multidisciplinary Sciences
Manu Suvarna, Alain Claude Vaucher, Sharon Mitchell, Teodoro Laino, Javier Perez-Ramirez
Summary: In this study, a transformer model is introduced to automate synthesis protocol extraction from heterogeneous catalysis literature, showcasing the potential of using automated synthesis protocol analysis to expedite literature review and analysis in the field. The research also highlights the lack of standardization in reporting protocols and provides guidelines for improving machine readability.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Florentine L. P. Veenstra, Therese Cibaka, Antonio J. Martin, Daniel Weigand, Joachim Kirchhoff, Vladimir Smirnov, Tsvetelina Merdzhanova, Javier Perez-Ramirez
Summary: Artificial leaves can reduce carbon dioxide into syngas using solar power and have the flexibility to control the composition of the syngas by adjusting the electrolyte flow, which is beneficial for decentralized production.
