Article
Energy & Fuels
Yi Yang, Haitao Zhang, Hongfang Ma, Weixin Qian, Qiwen Sun, Weiyong Ying
Summary: The effects of alkali metal promoters on high-temperature Fischer-Tropsch synthesis catalysts were investigated. The alkali metals donated electrons to iron species, promoting CO dissociative adsorption and suppressing hydrogen adsorption. This led to an increase in selectivity to light olefins. The content of e'-Fe2.2C increased with increasing basicity of the catalyst surface, which enhanced the C-C coupling ability and chain growth.
Article
Chemistry, Physical
Deizi Peron, Alan J. Barrios, Alan Taschin, Iulian Dugulan, Carlo Marini, Giulio Gorni, Simona Moldovan, Siddardha Koneti, Robert Wojcieszak, Joris W. Thybaut, Mirella Virginie, Andrei Y. Khodakov
Summary: The study found that antimony and tin have strong promoting effects on silica supported iron Fischer-Tropsch catalysts, significantly increasing the reaction rate and improving catalyst stability. The addition of these elements through impregnation can increase the intrinsic activity of iron surface sites by 7-10 times without affecting iron dispersion.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Physical
Tobias F. Kimpel, Jin-Xun Liu, Wei Chen, Robert Pestman, Emiel J. M. Hensen
Summary: Through IR spectroscopy and DFT calculations, it has been discovered that in the Fischer-Tropsch reaction, Mn promotes a silica-supported Co catalyst with a MnO layer covering the Co surface, activating adsorbed CO through reaction with an oxygen vacancy. This results in higher activity, higher CHx coverage, increased C5+ selectivity, and decreased CH4 selectivity. Increasing pressure amplifies the selectivity differences. However, above around 4 bar, the addition of Mn decreases C5+ selectivity, possibly due to its promotion of C-O bond dissociation but not chain growth. Migration of formed monomers for chain growth on the Co surface may be hindered by high CO coverage, especially at high pressure.
JOURNAL OF CATALYSIS
(2023)
Review
Chemistry, Applied
Renyang Zheng, Zaiku Xie
Summary: The sustainable development of the chemical industry requires novel and efficient catalysts and catalytic processes, especially eco-friendly and intrinsically safe processes. In-situ characterization of catalytic performance is of great significance for a comprehensive study on the structure-performance relationship of catalysts. Realizing full life cycle characterization of heterogeneous catalysts under industrial conditions remains a great challenge.
CHINESE JOURNAL OF CATALYSIS
(2021)
Article
Chemistry, Inorganic & Nuclear
Meaghan M. Deegan, Jonas C. Peters
Summary: The article describes the synthesis of Fe-CS complexes and the possibility of further producing Fe-carbynes. Strategies for achieving C-S bond cleavage from these complexes are discussed, as well as the limitations that have so far prevented the generation of terminal Fe-carbide in this system.
Article
Chemistry, Physical
Mikhail Shipilin, David Degerman, Patrick Lomker, Christopher M. Goodwin, Gabriel L. S. Rodrigues, Michael Wagsta, Joergen Gladh, Hsin-Yi Wang, Andreas Stierle, Christoph Schlueter, Lars G. M. Pettersson, Anders Nilsson, Peter Amann
Summary: In this study, the effect of pressure, temperature, time, and gas feed composition on the growth dynamics of iron-carbon phases was investigated. The details of iron surface carburization and product formation under realistic conditions were revealed using a combination of experimental and theoretical approaches. This research provides important insights into the relationship between the catalyst's surface and the reaction.
Article
Chemistry, Physical
Mikhail Shipilin, David Degerman, Patrick Loemker, Christopher M. Goodwin, Gabriel L. S. Rodrigues, Michael Wagstaffe, Jorgen Gladh, Hsin-Yi Wang, Andreas Stierle, Christoph Schlueter, Lars G. M. Pettersson, Anders Nilsson, Peter Amann
Summary: This study investigates the detailed mechanism of carbide formation on iron-based catalysts and the effect of reaction conditions on the catalyst surface state through experiments and theoretical calculations.
Article
Energy & Fuels
Shupeng Guo, Zhongyi Ma, Jungang Wang, Bo Hou, Litao Jia, Baojun Wang, Debao Li
Summary: The synergistic promotion effect of Ru and Ba in Co/Al2O3 catalyst achieved higher CO conversion and lower CH4 selectivity, compared to unmodified or single additive modified catalyst. The influences of other alkali earth metal additives were also similar to that of Ba in promoting FTS reaction on Co-Ru catalysts.
Article
Chemistry, Physical
Xiaoxue Han, Qiao Zhao, Huiyong Gong, Chongyang Wei, Jing Lv, Yue Wang, Mei-yan Wang, Shouying Huang, Xinbin Ma
Summary: In this study, Fe-oxide interfaces were constructed to investigate their effect on phase transformation and Fischer-Tropsch synthesis (FTS) performance. By correlating performance to the composition of iron species, the crucial role of Fe2.2C in high CO conversion and C5+ productivity has been confirmed. Furthermore, a heterogeneous spatial distribution of iron carbides and oxides induced by Fe-oxide interfaces was observed. This study provides insights for iron carbides formation and stability by modulating interfaces, which guides the further development of Fe-based FTS catalysts.
Article
Chemistry, Multidisciplinary
Meng Cui, Qingli Qian, Jingjing Zhang, Ying Wang, Bernard Baffour Asare Bediako, Huizhen Liu, Buxing Han
Summary: The study presents the production of liquid fuel from CO2 hydrogenation by coupling homogeneous RuCl3 and heterogeneous Ru-0 catalysts at the lowest reported temperature (180 degrees C) and achieving the highest C5+ selectivity to date (71.1%). The synergy of homogeneous and heterogeneous catalysis is identified as the key factor for the outstanding performance.
Article
Chemistry, Applied
Lilia Sineva, Ekaterina O. Gorokhova, Kirill O. Gryaznov, Ilya S. Ermolaev, Vladimir Z. Mordkovich
Summary: The use of zeolite-containing Co catalysts in liquid hydrocarbon transformations during Fischer-Tropsch synthesis demonstrated a decrease in the average molecular weight of the products without increasing methane selectivity. The introduction of zeolites cleared the catalyst pore system of heavier hydrocarbons, suggesting a potential role in controlling product composition over hybrid catalysts.
Article
Energy & Fuels
Mingquan Li, Aqsa Noreen, Yajie Fu, Cederick Cyril Amoo, Yujia Jiang, Xu Sun, Peng Lu, Ruiqin Yang, Chuang Xing, Shurong Wang
Summary: The study focuses on the direct synthesis of higher olefins (C5+) from syngas using a novel Fe@Na-ZSM-5 composite catalyst, achieving a selectivity of 70% olefins in gasoline. The promotion by Na ions enhances the formation of Fe5C2 phases, facilitating C-C coupling and increasing gasoline and olefins selectivity. Na type zeolite (Na-Zeolite) serves as a unique Na electron promoter, contributing significantly to the development of heterogeneous catalysts and functional materials.
Article
Chemistry, Multidisciplinary
Zhenpu Lu, Ran Luo, Sai Chen, Donglong Fu, Guodong Sun, Zhi-Jian Zhao, Chunlei Pei, Jinlong Gong
Summary: This study describes the effect of calcium on the propane dehydrogenation catalyst and finds that calcium can enhance the activity and selectivity of the platinum-tin catalyst by promoting the formation of tin and a highly reactive and sintering-resistant platinum-tin alloy.
Article
Multidisciplinary Sciences
lgor Levchenko, Shuyan Xu, Oleg Baranov, Kateryna Bazaka
Summary: Inhospitable and remote locations such as deserts, islands, and outer space offer unique opportunities for science, economy, and geopolitics, but the stable supply of energy is a critical challenge due to transportation difficulties and costs. This essay explores the advantages and challenges of integrating Fischer-Tropsch, artificial photosynthesis, and plasma catalysis into a self-contained system for energy harvesting, storage, and utilization.
Article
Chemistry, Multidisciplinary
Lili Lin, Yuzhen Ge, Hongbo Zhang, Meng Wang, Dequan Xiao, Ding Ma
Summary: Heterogeneous catalytic processes are crucial for producing fuels and chemicals in the chemical industry, and the addition of water in the aqueous phase or adsorbed micro water environment can enhance the performance of heterogeneous catalysts and create novel catalytic conversion routes.
Editorial Material
Chemistry, Multidisciplinary
Iris C. ten Have, Robin Y. van den Brink, Stephane C. Marie-Rose, Florian Meirer, Bert M. Weckhuysen
Summary: This article introduces a method that utilizes waste particles from biomass gasification as solid catalysts to produce high-value chemicals from mixtures of H-2, CO, and CO2. The catalyst material consists of nanoparticles composed of iron carbides, iron metal, and alkali elements, such as sodium and potassium. This approach demonstrates the application of the concept of materials circularity.
Article
Chemistry, Multidisciplinary
Iris C. ten Have, Robin Y. van den Brink, Stephane C. Marie-Rose, Florian Meirer, Bert M. Weckhuysen
Summary: Gasification is a process that converts solid waste into gaseous feedstock. This study investigates the possibility of using waste gasification solid residue as a catalyst for producing light olefins. Experimental results show that the catalyst can convert biomass-derived syngas into methane and olefins.
Article
Chemistry, Physical
Yohei Uemura, Ahmed S. M. Ismail, Sang Han Park, Soonnam Kwon, Minseok Kim, Hebatalla Elnaggar, Federica Frati, Hiroki Wadati, Yasuyuki Hirata, Yujun Zhang, Kohei Yamagami, Susumu Yamamoto, Iwao Matsuda, Ufuk Halisdemir, Gertjan Koster, Christopher Milne, Markus Ammann, Bert M. Weckhuysen, Frank M. F. de Groot
Summary: In this study, the photoexcited state of a hematite thin film was investigated using X-ray absorption spectroscopy, and the 200 fs decay time of the hole state in the valence band was observed.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Bas Terlingen, Ramon Oord, Mathieu Ahr, Eline M. Hutter, Coert van Lare, Bert M. Weckhuysen
Summary: The oxychlorination reaction of methane has the potential to achieve high conversion rates and selectivities. By replacing a portion of Eu3+ with La3+, the catalyst design of EuOCl can be improved to enhance CH3Cl yield and selectivity, while reducing catalyst and separation costs.
Article
Chemistry, Applied
Xin Li, Kang Hu, Yizhe Huang, Qingqing Gu, Yuwen Chen, Bing Yang, Rongliang Qiu, Wenhao Luo, Bert M. Weckhuysen, Kai Yan
Summary: In this study, biomass waste ferns contaminated by iron mines were used to fabricate a high-performance Fe single-atom catalyst (FeSAC), which showed excellent efficiency in the photodegradation of various antibiotics. These findings provide a new approach for the efficient utilization of biomass waste in pollutant control.
JOURNAL OF ENERGY CHEMISTRY
(2022)
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)
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
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
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, 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
Ellen B. Sterk, Anne-Eva Nieuwelink, Matteo Monai, Jaap N. Louwen, Eelco T. C. Vogt, Ivo A. W. Filot, Bert M. Weckhuysen
Summary: Nickel metal nanoparticles exhibit structure sensitivity in the catalytic conversion of CO2 to CH4, with the Ni(110) facet showing the highest activity. The dissociation of H2CO* to CH2* and O* on this facet is identified as the most critical elementary reaction step. Simulation calculations reveal a correlation between the activity of nickel metal nanoparticles and their size.
Article
Chemistry, Multidisciplinary
Sophie H. van Vreeswijk, Matteo Monai, Ramon Oord, Joel E. Schmidt, Andrei N. Parvulescu, Irina Yarulina, Lukasz Karwacki, Jonathan D. Poplawsky, Bert M. Weckhuysen
Summary: The introduction of magnesium as a cationic metal in the catalytic conversion of methanol to valuable hydrocarbon molecules using zeolite materials has been found to change the properties of the zeolite and improve the catalytic performance. Atom probe tomography and nanoscale analysis techniques were used to reveal the aggregation and distribution of magnesium within zeolite materials. The unique coking mechanism and evidence for the formation of polyaromatic compounds in zeolite SSZ-13 were also discovered.
