Article
Chemistry, Physical
M. Gambino, A. E. Nieuwelink, F. Reints, M. Vesely, M. Filez, D. Ferreira Sanchez, D. Grolimund, N. Nesterenko, D. Minoux, F. Meirer, B. M. Weckhuysen
Summary: Using a correlative microscopy approach, this study investigated the spatial heterogeneities in artificially deactivated catalysts and compared the impact of metal contaminants on catalyst acidity and pore accessibility. The findings suggest that in addition to metal distribution, hydrothermal degradation also plays a role in dealumination and acidity drop in ECATs. Fe contamination must also be considered for its effect on matrix accessibility.
JOURNAL OF CATALYSIS
(2021)
Article
Engineering, Environmental
Martin Rodriguez-Fragoso, Shantal Zavala-Salazar, Miriam Moreno-Montiel, Christian Bouchot, Octavio Elizalde-Solis, Edgar Ramirez-Jimenez
Summary: An 8-lumps kinetic model based on feedstock composition is proposed. The model is fitted using a sensitivity analysis to identify reaction pathways contributing significantly to the desired products, resulting in improved fitting. It considers commonly used lumps in the industry, making it useful. An uncertainty analysis is performed to provide a probability bandwidth for experimental data and acknowledge possible errors. The model can predict behavior of different feedstocks using a single set of kinetic parameters differentiated by a deactivation factor.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Green & Sustainable Science & Technology
Ashish Pathak, Mohan S. Rana, Meena Marafi, Richa Kothari, Piyush Gupta, V. V. Tyagi
Summary: In this study, we critically analyzed the potential of reusing spent fluid cracking catalysts (SFCC) as raw materials for synthesizing zeolites, and discussed the challenges and prospects of this process.
SUSTAINABLE MATERIALS AND TECHNOLOGIES
(2023)
Article
Chemistry, Physical
Fan Lin, Mengze Xu, Karthikeyan K. Ramasamy, Zhenglong Li, Jordan Lee Klinger, Joshua A. Schaidle, Huamin Wang
Summary: The article discusses the challenges faced by biomass conversion technologies, specifically in terms of catalyst deactivation and mitigation. It highlights the unique properties of biomass-derived feedstocks that cause catalyst deactivation and provides information on potential mitigation approaches to guide the design of robust catalysts and processes for biomass conversion.
Article
Chemistry, Multidisciplinary
Yuhao Wang, Genyuan Wang, Lars I. van der Wal, Kang Cheng, Qinghong Zhang, Krijn P. de Jong, Ye Wang
Summary: The catalytic performance of composite catalysts is influenced by the interaction between components and the migration of metals. Different metals exhibit different migration behavior towards zeolite, affecting the selectivity of hydrocarbon products.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Review
Energy & Fuels
D. E. Adanenche, A. Aliyu, A. Y. Atta, B. J. El-Yakubu
Summary: The catalysts used for residue fluid catalytic cracking must possess various qualities to withstand the challenges posed by heavy feedstocks and their high concentration of harmful heteroatom poisons. This study discusses the differences between conventional and contemporary fluid catalytic cracking, highlighting the importance of effectively mitigating the harmful effects of nickel and vanadium through the use of antimony and boron compounds. It also presents new insights into nickel and vanadium poisoning mechanisms.
Article
Chemistry, Physical
Takaki Mizuno, Hiroshi Yamazaki, Yusuke Takamiya, Hiroki Hasegawa, Chisuzu Tanaka, Tomohiro Mitsui
Summary: The effects of fluid catalytic cracking (FCC) catalyst binder type on catalytic properties were investigated. SiO2 and Al2O3 were used as binders for the FCC catalysts. The SiO2 binder catalyst showed higher propylene yield compared to the Al2O3 binder catalyst when the ZSM-5 additive was blended. The SiO2 binder catalyst also exhibited higher SAmicro and different acid properties after steaming.
APPLIED CATALYSIS A-GENERAL
(2023)
Article
Chemistry, Physical
Aleksei Vjunov, Karl C. Kharas, Vasileios Komvokis, Amy Dundee, Claire C. Zhang, Bilge Yilmaz
Summary: This study presents a CO promoter design strategy that can increase CO conversion efficiency without the need for additional precious metal loading, by focusing on the support material architecture. The results show a significant reduction in Pt cost and usage rate compared to current industry-standard designs.
Article
Chemistry, Physical
Yong Yang, Chaowei Liu, Xueli Ma, Zixuan Zu, Yi Su, Hongwei Li, Dong Ji
Summary: This study investigates the effects of metal contamination, specifically nickel, vanadium, and iron, on fluid catalytic cracking (FCC) catalysts. The results show that each metal has different destructive effects on the catalyst, with vanadium having the highest deactivation effect, while iron reduces the acidic sites. Multiple metal deposition leads to more serious performance issues.
Review
Chemistry, Physical
Minghui Li, Yaning Yang, Dailiang Yu, Wenwen Li, Xin Ning, Rui Wan, Hongjie Zhu, Junjie Mao
Summary: This review presents the recent advances in encapsulated catalysts since 2016, discussing the effects of encapsulation structure on performance and key factors controlling the structure of encapsulated catalysts.
Article
Chemistry, Multidisciplinary
Yitao Liao, Tao Liu, Xiaohui Du, Xionghou Gao
Summary: The study found that nodules form on the catalyst surface when the iron concentration exceeds 7,400 μg/g, and iron deposition leads to a significant decrease in surface area and pore volume, as well as a decrease in catalytic efficiency.
FRONTIERS IN CHEMISTRY
(2021)
Article
Biotechnology & Applied Microbiology
Eki Tina Aisien, Ifechukwude Christopher Otuya, Felix Aibuedefe Aisien
Summary: The study focused on the pyrolysis of waste polypropylene plastic using a batch reactor with varying reaction temperatures and catalyst ratios. The results showed that the catalyst, reaction temperatures, and catalyst to plastic ratio all had significant impact on the yield and composition of the pyrolysis products.
ENVIRONMENTAL TECHNOLOGY & INNOVATION
(2021)
Review
Chemistry, Physical
Minghui Li, Yaning Yang, Dailiang Yu, Wenwen Li, Xin Ning, Rui Wan, Hongjie Zhu, Junjie Mao
Summary: This review highlights the recent advances in the preparation and application of encapsulated catalysts since 2016. Encapsulation strategies, which involve coating active species with protective shells, have been proven to enhance catalytic performance and present opportunities and challenges for further research.
Article
Engineering, Environmental
Jiawei Bian, Bohan Wang, Ximing Niu, Hai Zhao, Hao Ling, Feng Ju
Summary: This study investigates the migration and emission characteristics of metal pollutants in fluid catalytic cracking (FCC) units. The migration rates of vanadium (V), nickel (Ni), and iron (Fe) are found to be relatively high, while other metals exhibit lower migration rates. The distribution of metals on catalysts significantly influences their mobility and the regeneration process affects catalyst attrition, resulting in discrepancies in metal particulate matter (PM) emissions.
JOURNAL OF HAZARDOUS MATERIALS
(2024)
Article
Energy & Fuels
Jiaxing Wang, Shuping Zhang, Dan Xu, Huiyan Zhang
Summary: Developing an efficient and inexpensive catalyst for the removal of tar is crucial in biomass gasification technology. In this study, a red mud/carbonaceous catalyst was prepared through in-situ carbothermal reduction and showed improved catalytic activity and stability. The catalyst achieved a tar conversion efficiency of 88.70% at a temperature of 700 degrees C and maintained 80.15% conversion after nine cycles.
Correction
Chemistry, Multidisciplinary
Matteo Monai, Marianna Gambino, Sippakorn Wannakao, Bert M. Weckhuysen
CHEMICAL SOCIETY REVIEWS
(2023)
Article
Chemistry, Multidisciplinary
Eduardo Solano, Jolien Dendooven, Davy Deduytsche, Nithin Poonkottil, Ji-Yu Feng, Maarten B. J. Roeffaers, Christophe Detavernier, Matthias Filez
Summary: This paper presents a multi-pronged approach that provides complementary information on the sintering of platinum nanoparticles at multiple length scales. The study reveals that the size evolution of individual nanoparticles depends on the number of coalescence events they undergo during their lifetime and that the probability of coalescence is strongly influenced by the nanoparticles' mesoscale environment. Additionally, it is found that nanoparticles with different crystallographic orientations exhibit different susceptibility to sintering.
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)
Editorial Material
Chemistry, Physical
Javier Perez-Ramirez, Bert M. Weckhuysen, Maria E. Southall
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Ian Byrnes, Lisa Magdalena Rossbach, Dag Anders Brede, Daniel Grolimund, Dario Ferreira Sanchez, Gert Nuyts, Viclav Cuba, Estela Reinoso-Maset, Brit Salbu, Koen Janssens, Deborah Oughton, Shane Scheibener, Hans -Christian Teien, Ole Christian Lind
Summary: This study investigated the biodistribution and adverse effects of uranium nanoparticle (UNP) suspensions and uranium reference (Uref) solutions on Daphnia magna. The results showed similar size distributions and acute effects between the two exposures. However, the uranium body burden was significantly greater in UNP-exposed daphnids, and the specific toxicity was higher in Uref exposure. High-resolution X-ray fluorescence elemental maps revealed uranium accumulation in various organs and tissues, including gills, hepatic ceca, intestinal lumen, heart, maxillary gland, and embryos. These findings contribute to the understanding of uranium and UNP toxicity and exposure characterization.
Article
Chemistry, Multidisciplinary
Alexandre C. Foucher, Shengsong Yang, Daniel J. Rosen, Renjing Huang, Jun Beom Pyo, Ohhun Kwon, Cameron J. Owen, Dario Ferreira Sanchez, Ilia I. Sadykov, Daniel Grolimund, Boris Kozinsky, Anatoly I. Frenkel, Raymond J. Gorte, Christopher B. Murray, Eric A. Stach
Summary: We developed a method to synthesize highly mono-disperse Cu-Pt alloy nanoparticles. These nanoparticles exhibited stability under redox conditions and displayed promising activity and stability for CO oxidation. The incorporation of Pt with Cu did not lead to rapid deactivation and degradation of the material as seen with other bimetallic systems. This work provides a synthesis route to control the design of Cu-Pt nanostructures and highlights the potential of these alloys for heterogeneous catalysis.
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
Shiyou Xing, Savannah Turner, Donglong Fu, Sophie van Vreeswijk, Yuanshuai Liu, Jiadong Xiao, Ramon Oord, Joachim Sann, Bert M. Weckhuysen
Summary: This study achieved CO2 hydrogenation on In2O3/H-ZSM-5 catalyst by coating a layer of S-1, overcoming catalyst deactivation caused by powder mixing and improving catalyst activity and lifetime. The S-1-coated catalyst showed enhanced performance under both nanoscale and microscale proximity.
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)
Correction
Chemistry, Multidisciplinary
Maximilian J. J. Werny, Jelena Zarupski, Iris C. C. ten Have, Alessandro Piovano, Coen Hendriksen, Nicolaas H. H. Friederichs, Florian Meirer, Elena C. C. Groppo, Bert M. M. Weckhuysen
Article
Chemistry, Multidisciplinary
Hongyu An, Jim de Ruiter, Longfei Wu, Shuang Yang, Florian Meirer, Ward van der Stam, Bert M. M. Weckhuysen
Summary: The activity and selectivity of a copper electrocatalyst during the electrochemical CO2 reduction reaction (eCO(2)RR) are influenced by the interplay between the local reaction environment, catalyst surface, and adsorbed intermediates. Raman spectroscopy with space and time resolution was used to investigate the distribution of adsorbed species on a copper electrode during eCO(2)RR. The results showed spatial heterogeneities in adsorbed species and the presence of CO-dominant and C-C dominant regions on the electrode surface. In situ micro-spectroscopic techniques are crucial for understanding the eCO(2)RR mechanism of working electrocatalyst materials.
Article
Chemistry, Physical
Alessia Broccoli, Luca Carnevale, Rafael Mayorga Gonzalez, Joren M. Dorresteijn, Bert M. Weckhuysen, Wouter Olthuis, Mathieu Odijk, Florian Meirer
Summary: Understanding mass transfer in solid catalysts, batteries, fuel cells, and adsorbents is crucial for improving their performance. We present a new method to evaluate the accessibility of functional porous materials at the single-particle level, using a multiplexed microfluidic device and a fluorescence microscope to assess the uptake of fluorescent molecules in porous particles.
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
Forestry
Paula Ballikaya, Ivano Brunner, Claudia Cocozza, Daniel Grolimund, Ralf Kaegi, Maria Elvira Murazzi, Marcus Schaub, Leonie C. Schoenbeck, Brian Sinnet, Paolo Cherubini
Summary: This study investigated the uptake and transport mechanisms of gold nanoparticles (Au-NPs) in European beech and Scots pine trees. The results showed that both tree species were capable of taking up and transporting Au-NPs to their stem. European beech exhibited higher uptake of Au-NPs, possibly due to its higher stomatal density and wood characteristics.
