Article
Chemistry, Physical
Luca Botti, Sebastian Meier, Ceri Hammond
Summary: This study investigates the catalytic conversion of glucose using Lewis acidic silicates in a continuous flow reactor with operando UV-vis spectroscopy. Transient absorption features related to glucose activation and conversion at various operational conditions are identified, and the deactivation of the stannosilicate catalyst is shown to affect the overall performance of the glucose upgrading reaction during continuous operation. The study highlights the nonuniform deactivation of the catalyst and its implications for improving the selectivity of catalysts for glucose upgrading.
Article
Chemistry, Physical
Mikalai A. Artsiusheuski, Jeroen A. van Bokhoven, Vitaly L. Sushkevich
Summary: The one-step valorization of natural gas is still a challenge, and converting methane to methanol via chemical looping over copper-containing zeolites seems to be a promising route. CuMFI is one of the earliest successful methods, but the structure of the active sites in CuMFI and the influence of copper loading and Si/Al ratio on the copper speciation are still not well understood. It has been found that the Cu/Al ratio determines the selectivity of methane conversion in CuMFI by controlling the structure of the active dicopper sites.
Article
Chemistry, Physical
Mikalai A. Artsiusheuski, Jeroen A. van Bokhoven, Vitaly L. Sushkevich
Summary: The one-step valorization of natural gas is a challenge, and converting methane to methanol via chemical looping over copper-containing zeolites shows promise. Research has found that the Cu/Al ratio determines the selectivity of methane conversion by controlling the structure of the active copper sites.
Article
Engineering, Environmental
Fabricio C. Tanaka, Carlos. R. F. Junior, Renan. S. Fernandes, Marcia R. de Moura, Fauze A. Aouada
Summary: This study investigated the morphological and thermal properties, as well as the swelling degree at different pH values of zeolite-based nanocomposites. The water-uptake in various swelling media was correlated with sorption and desorption profiles of diquat, showing improved herbicide-matrix interaction with the addition of zeolite. The pH variation of the swelling media might have influenced the elasticity of the nanocomposite chains, impacting the release rate.
JOURNAL OF POLYMERS AND THE ENVIRONMENT
(2021)
Article
Spectroscopy
Smita Verma, Velayutham Ravichandiran, Nihar Ranjan
Summary: A selective fluorescence sensor for carbonate ions has been developed in this study, which can rapidly detect low concentrations of carbonate ions. Experimental results demonstrate direct interaction between the sensor and carbonate ions, with potential implications for disease prevention and toxicity assessment.
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
(2021)
Article
Chemistry, Multidisciplinary
Alberto Gimenez-Gomez, Benjamin Rollins, Andrew Steele, Helen Holzel, Nicolo Baggi, Kasper Moth-Poulsen, Ignacio Funes-Ardoiz, Diego Sampedro
Summary: Solar energy utilization has gained attention for its abundance and renewability. Developing energy storing compounds that capture and release solar energy on demand is a potential solution. These compounds undergo a photochemical transformation, storing solar energy in high-energy photoisomers. While the photoisomerization of MOlecular Solar Thermal (MOST) systems has been extensively studied, the back-conversion using heterogeneous catalysts is still underexplored. In this study, the performance of 27 catalysts in releasing stored energy in a Norbornadiene/Quadricyclane MOST system is compared using UV-Vis spectroscopy. The findings provide insights for the development of effective catalysts in MOST systems and highlight the importance of further investigation on heterogeneous catalysis.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Physical
Pavol Tisovsky, Klaudia Csicsai, Jana Donovalova, Robert Sandrik, Jozef Kozisek, Anton Gaplovsky
Summary: Zn(II) complexes were synthesized using L-a and L-b, with the Z-isomers isolated from the reaction mixture. The structure of these complexes was determined by NMR spectroscopy and X-ray diffraction analysis. The Z-isomers of complexes can undergo changes in the hydrazo = azo equilibrium through light-stimulated photoreactions.
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
(2021)
Review
Multidisciplinary Sciences
Sophie H. van Vreeswijk, Bert M. Weckhuysen
Summary: This paper reviews advanced and emerging analytical methods for studying zeolite properties and working behavior, highlighting the importance of these materials in various applications and the necessity of understanding them for transitioning into a more circular society. New techniques like atom probe tomography and confocal fluorescence microscopy, along with established methods such as nuclear magnetic resonance and X-ray diffraction, have contributed to a deeper understanding of zeolite materials. In situ/operando analysis has provided new insights into reaction and deactivation mechanisms of zeolites under working conditions.
NATIONAL SCIENCE REVIEW
(2022)
Review
Agronomy
Andres Perez-San Martin, Frutos C. Marhuenda-Egea, Maria Angeles Bustamante, Gustavo Curaqueo
Summary: This review critically analyzes and updates the chemical spectroscopy methods for evaluating the transformation of organic matter in composting, and discusses their potential applications in optimizing compost quality for agricultural use.
Article
Chemistry, Physical
J. J. Erik Maris, Donglong Fu, Florian Meirer, Bert M. Weckhuysen
Summary: This article reviews the development of spatial and temporal characterization of nanoporous solids using single-molecule localization microscopy, illustrating how this approach can be used to track molecular diffusion and reaction behaviors in nanoporous solids.
ADSORPTION-JOURNAL OF THE INTERNATIONAL ADSORPTION SOCIETY
(2021)
Article
Biophysics
Narges Ashrafi, Behzad Shareghi, Sadegh Farhadian, Mansoore Hosseini-Koupaei
Summary: This study investigated the effect of polyamine on the compound and function of lysozyme using UV-Visible and fluorescence spectroscopy as well as simulation method. The results showed that increasing polyamine concentration reduced the intrinsic quenching fluorescence of lysozyme and altered its secondary and tertiary structures. Polyamine also inhibited the enzymatic activity of lysozyme.
COLLOIDS AND SURFACES B-BIOINTERFACES
(2022)
Article
Chemistry, Physical
Faisal H. Alshafei, Youngkyu Park, Stacey I. Zones, Mark E. Davis
Summary: ERI-type molecular sieves with varying Si/Al and Si/T-atom ratios showed improved performance in the methanol-to-olefins reaction. They exhibited higher ethylene-to-propylene ratios compared to other zeolites, while SAPO-17 samples had a higher C-4+ fraction. The differences in product distributions were attributed to the slower maturation of aromatic hydrocarbon-pool species and the presence of aromatics with bulky alkyl-groups in SAPO-17 samples.
JOURNAL OF CATALYSIS
(2021)
Article
Chemistry, Physical
Xiangrong Li, Xuezhen Wang, Hongyi Liu, Yanru Peng, Yunhui Yan, Tianjun Ni
Summary: The study investigated the binding of eight classic flavonoids to gamma-globulin, revealing different binding affinities and main interactions such as electrostatic forces, hydrogen bonding, and hydrophobic interactions. The interaction between flavonoids and gamma-globulin alters the protein structure, particularly affecting the secondary structure of the protein.
JOURNAL OF MOLECULAR STRUCTURE
(2021)
Article
Chemistry, Multidisciplinary
Xiangkun Wu, Zihao Zhang, Zeyou Pan, Xiaoguo Zhou, Andras Bodi, Patrick Hemberger
Summary: In this study, the experimental detection of methylketene as the precursor of ethylene on HZSM-5 was reported, providing evidence for the computationally predicted ketene-to-ethylene reaction pathway.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Nikolaos Nikolopoulos, Robin G. Geitenbeek, Gareth T. Whiting, Bert M. Weckhuysen
Summary: One of the main challenges for the chemical industry in the future is to convert low-grade industrial waste into valuable materials, such as waste flotation tailings into solid acid catalysts. This study found that impurities in waste-derived zeolites can affect their physicochemical properties and catalytic performance.
JOURNAL OF CATALYSIS
(2021)
Correction
Chemistry, Multidisciplinary
Matteo Monai, Marianna Gambino, Sippakorn Wannakao, Bert M. Weckhuysen
CHEMICAL SOCIETY REVIEWS
(2023)
Article
Multidisciplinary Sciences
Guusje Delen, Matteo Monai, Katarina Stanciakova, Bettina Baumgartner, Florian Meirer, Bert M. Weckhuysen
Summary: Researchers have discovered that the sorption and conversion of gaseous molecules on the surface of functional materials preferentially occur on specific undercoordinated high-index surface sites. By combining in situ PiFM with DFT calculations, they have studied the site-specific sorption and conversion of formaldehyde on faceted ZIF-8 microcrystals and observed preferential adsorption on high-index planes. They have also visualized unsaturated nanodomains and found structure sensitive conversion mediated by Lewis acidity on defective ZIF-8 crystals.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Il Son Khan, Luis Garzon-Tovar, Toni Grell, Genrikh Shterk, Jose Cerrillo, Tuiana Shoinkhorova, Juan C. Navarro, Faisal Alahmadi, Angel Sousa, Anastasiya Bavykina, Daria Poloneeva, Mustafa Caglayan, Stephanie Terruzzi, Javier Ruiz-Martinez, Nikolay Kosinov, Valentina Colombo, Jorge Gascon
Summary: The use of metal-organic frameworks (MOFs) as precursors for heterogeneous catalysts has attracted much attention. Steaming during the controlled decomposition of MOFs leads to the formation of smaller, well-dispersed metal nanoparticles, resulting in more efficient catalysts. This study demonstrates the benefits of steam addition, including improved phase composition control and catalyst activity, for CO2 hydrogenation.
Editorial Material
Chemistry, Physical
Javier Perez-Ramirez, Bert M. Weckhuysen, Maria E. Southall
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Laurens D. B. Mandemaker, Christia Jabbour, Nikolaos Nikolopoulos, Joren M. Dorresteijn, Miguel Rivera-Torrente, Bert M. Weckhuysen
Summary: The growth mechanisms and molecular phenomena of UiO-67, UU-1, and ZIF-8 metal-organic framework (MOF) films on transparent substrates are studied using transmission-based characterization. UiO-67 follows a Volmer-Weber growth mechanism with assistance from solution-grown seeds. UU-1 exhibits fiber-like morphology and inter-fiber macroporosity, while ZIF-8 shows a similar Volmer-Weber growth mode. CO probe molecule adsorption FT-IR spectroscopy reveals the effects of methanol exposure, with UiO-67 becoming inaccessible to CO, UU-1 undergoing a topotactic transformation, and ZIF-8 remaining stable with impurity removal. This approach opens new possibilities for studying other film materials using transmission-based spectroscopy.
ADVANCED MATERIALS INTERFACES
(2023)
Article
Chemistry, Physical
Pierfrancesco Ticali, Sara Morandi, Genrikh Shterk, Samy Ould-Chikh, Adrian Ramirez, Jorge Gascon, Sang-Ho Chung, Javier Ruiz-Martinez, Silvia Bordiga
Summary: The present work investigates the application of a previously studied PdZn/ZrO2+SAPO-34 bifunctional catalyst for CO2 conversion. High activity and selectivity for propane were observed. The results obtained from NAP-XPS measurements and CO adsorption at liquid-nitrogen temperature (LNT) followed by FT-IR spectroscopy provide insights into the behavior of the catalyst. Fresh, used, and regenerated states of the catalyst were characterized, revealing interactions between different components and the formation of new species in the catalyst framework.
APPLIED CATALYSIS A-GENERAL
(2023)
Article
Chemistry, Multidisciplinary
Qingpeng Cheng, Guanna Li, Xueli Yao, Lirong Zheng, Junhu Wang, Abdul-Hamid Emwas, Pedro Castano, Javier Ruiz-Martinez, Yu Han
Summary: This study presents a facile synthesis strategy for incorporating more Fe into the zeolite framework. The Fe-ZSM-5 catalyst prepared using this method has three times as many active sites as conventional Fe-ZSM-5, leading to a record-high C-1 oxygenate yield in the selective oxidation of CH4.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Thuy T. Le, Wei Qin, Ankur Agarwal, Nikolaos Nikolopoulos, Donglong Fu, Matthew D. Patton, Conan Weiland, Simon R. Bare, Jeremy C. Palmer, Bert M. Weckhuysen, Jeffrey D. Rimer
Summary: This study reveals that the presence of a catalytically inactive siliceous exterior rim on ZSM-5 particles can significantly reduce diffusion limitations, leading to an improved catalyst lifetime. The synthesis of Si-zoned ZSM-5 catalysts improves the diffusion properties of the catalyst. Operando ultraviolet-visible light diffuse reflectance spectroscopy shows a substantial reduction in external coking among Si-zoned samples. Molecular dynamics simulations demonstrate that there are significantly reduced transport limitations in the zoned regions, which contributes to the improved catalyst activity of Si-zoned zeolites compared to ZSM-5 with a homogeneous acid-site distribution.
Article
Chemistry, Multidisciplinary
Rushana Khairova, Sarah Komaty, Alla Dikhtiarenko, Jose Luis Cerrillo, Sudheesh Kumar Veeranmaril, Selvedin Telalovic, Antonio Aguilar Tapia, Jean-Louis Hazemann, Javier Ruiz-Martinez, Jorge Gascon
Summary: Metal encapsulation in zeolitic materials through one-pot hydrothermal synthesis is an attractive technique to prepare zeolites with high metal dispersion. Metallosiloxanes are used as an alternative metal precursor, leading to quantitative metal loading and high dispersion. Fe-MFI zeolites synthesized using this method exhibit high catalytic activity in NH3-mediated selective catalytic reduction (SCR) of NOx.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
J. J. Erik Maris, Luke A. Parker, Katarina Stanciakova, Nikolaos Nikolopoulos, Koen M. H. Berendsen, Alfons van Blaaderen, Florian Meirer, Freddy T. Rabouw, Bert M. Weckhuysen
Summary: In this study, we used confocal laser scanning microscopy to investigate the molecular accessibility and diffusion of a small fluorescent dye molecule, resorufin, in the hierarchical, anisotropic pore structure of large zeolite-beta crystals. Our findings revealed that protonated resorufin exhibits strong fluorescence when confined within zeolite micropores, enabling fluorescence microimaging experiments. Through our experiments, we were able to characterize the pore space and quantify the diffusion coefficient in the straight pores of zeolite-beta. We also observed that diffusion is impeded when crossing the boundaries between zeolite subunits.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Florian Zand, Suzanne J. T. Hangx, Christopher J. Spiers, Peter J. van den Brink, James Burns, Matthew G. Boebinger, Jonathan D. Poplawsky, Matteo Monai, Bert M. Weckhuysen
Summary: Understanding and controlling the structure and composition of nanoparticles in supported metal catalysts are crucial for improving chemical processes. Atom probe tomography (APT) is a powerful tool for three-dimensional chemical imaging of materials with nanometer resolution. However, APT has not been used for mesoporous oxide-supported metal catalysts due to sample fracture. In this study, we developed a high-pressure resin impregnation strategy to overcome this issue and successfully applied APT to high-porous supported Pd-Ni catalyst materials active in CO2 hydrogenation. Our results demonstrate the capability of APT to quantitatively assess the size, composition, and metal distribution of nanoparticles in industrial catalysts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Teng Li, Sang-Ho Chung, Stefan Nastase, Adrian Galilea, Yan Wang, Ildar Mukhambetov, Moussa Zaarour, Juan Carlos Navarro de Miguel, Jurjen Cazemier, Abhay Dokania, Liliana Panarone, Jorge Gascon, Luigi Cavallo, Javier Ruiz-Martinez
Summary: In this study, two H-ZSM-5 zeolites with different aluminum distributions were compared, and it was found that aluminum enrichment closer to the surface leads to more paired acid sites and enhanced catalytic activity. Furthermore, this aluminum distribution accelerates cascade reactions to produce aromatics and improves their diffusion out of the zeolite. By exploiting this feature, hollow zeolites were successfully fabricated, combining optimized active sites and improved diffusion and confinement properties to achieve the highest capacity for aromatic production.
Article
Chemistry, Physical
Mustafa Caglayan, Abdallah Nassereddine, Stefan-Adrian F. Nastase, Antonio Aguilar-Tapia, Alla Dikhtiarenko, Sang-Ho Chung, Genrikh Shterk, Tuiana Shoinkhorova, Jean-Louis Hazemann, Javier Ruiz-Martinez, Luigi Cavallo, Samy Ould-Chikh, Jorge Gascon
Summary: Tungsten is a promising metal with higher thermal stability for replacing molybdenum in methane dehydroaromatization (MDA) catalysis. However, the MDA activity of W-ZSM-5 catalysts is lower than their Mo counterpart. In order to understand the differences in catalytic activity, thorough investigations are conducted on the dispersion and distribution of W sites on the zeolite.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Mark J. J. Mangnus, Vincent R. M. Benning, Bettina Baumgartner, P. Tim Prins, Thomas P. van Swieten, Ayla J. H. Dekker, Alfons van Blaaderen, Bert M. Weckhuysen, Andries Meijerink, Freddy T. Rabouw
Summary: This study investigates the influence of solvent and gas environments on the photoluminescence (PL) properties of lanthanide-doped nanocrystals, and explains the changes in PL spectrum and excited-state lifetimes using energy transfer mediated by molecular vibrations. EVET-mediated quenching holds promise for probing the local chemical environment of nanocrystals dispersed in a liquid or exposed to gaseous molecules.
Article
Chemistry, Multidisciplinary
Rushana Khairova, Sarah Komaty, Alla Dikhtiarenko, Jose Luis Cerrillo, Sudheesh Kumar Veeranmaril, Selvedin Telalovic, Antonio Aguilar Tapia, Jean-Louis Hazemann, Javier Ruiz-Martinez, Jorge Gascon
Summary: Encapsulating metal in zeolitic materials through one-pot hydrothermal synthesis is an attractive technique to prepare zeolites with high metal dispersion. This study introduces the use of metallosiloxanes as an alternative metal precursor and demonstrates their effectiveness in achieving quantitative metal loading and high dispersion. Fe-MFI zeolites obtained through this method exhibit high catalytic activity and good tolerance in the NH3-mediated SCR of NOx.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
