Article
Chemistry, Physical
Elsa Koninckx, Pedro S. F. Mendes, Joris W. Thybaut, Linda J. Broadbelt
Summary: This study provides a complete and detailed mechanism of heterogeneous Ni-catalyzed oligomerization on solid acids for efficient production of desired products. By combining experimental, computational, and modeling studies, the bifunctional effects of nickel and acid sites on ethylene oligomerization are elucidated, highlighting the potential for optimal catalyst design. The selective oligomerization of ethylene to light, linear alkenes via the Cossee-Arlman mechanism by Ni2+ and further catalysis by Bronsted H+ sites are systematically discussed, emphasizing the importance of reaction conditions and catalyst properties.
APPLIED CATALYSIS A-GENERAL
(2021)
Article
Chemistry, Physical
Adrian Martinez Gomez-Aldaravi, Cecilia Paris, Manuel Moliner, Cristina Martinez
Summary: Diverse Ni-zeolites with different physico-chemical properties and Ni speciation have been designed to study their influence on ethylene oligomerization. Different particle sizes, Si/Al ratios, and Ni-incorporation strategies have been used to synthesize Ni-containing medium-pore MFI and large-pore BEA zeolites. Ni2+ and NiO nanoclusters are found inside the zeolitic pores, depending on the incorporation method. The presence of Ni2+ mainly determines olefin oligomerization under near-ambient pressures, while crystal size, acidity, and Ni incorporation methodology play key roles under high-pressure reaction conditions.
JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Inorganic & Nuclear
Na Zhang, Rui Jin, Guoliang Mao, Jinyan Tan, Liduo Chen, Cuiqin Li, Jun Wang
Summary: Metal organic frameworks UiO-66-NH2 were modified by reacting with amino groups to form a pyridineimine ligand for nickel catalyst. The catalytic performance in ethylene oligomerization was influenced significantly by catalyst structure, reaction temperature, Al/Ni molar ratio, and reaction pressure. Optimal conditions yielded a catalytic activity of 3.76 x 10(5) g.(mol Ni.h)(-1) with 75.94% selectivity towards butene at 25 degrees C, Al/Ni molar ratio of 1000, and reaction pressure of 1.2 MPa.
INORGANICA CHIMICA ACTA
(2022)
Article
Chemistry, Inorganic & Nuclear
Giyjaz E. Bekmukhamedov, Aleksandr V. Sukhov, Aidar M. Kuchkaev, Airat M. Kuchkaev, Khasan R. Khayarov, Alexey B. Dobrynin, Vasily M. Babaev, Dmitry G. Yakhvarov
Summary: This study compares the catalytic activity of nickel(II) complexes with different 1,10-phenanthroline ligands in the homogeneous ethylene oligomerization process. The results show that the catalytic activity and selectivity of the catalysts can be significantly influenced by the chemical structure of the ligands.
Article
Chemistry, Applied
Miria Terra da Costa, Eric Francis Lopes, Robson S. Oliboni, Diogo S. Ludtke, Osvaldo L. Casagrande Jr, Rafael Stieler
Summary: A new synthetic route to arylchalcogenyl-sulfonate ligands and the synthesis and ethylene reactivity of two nickel complexes are reported. The complexes' minimum energy structures were determined by density functional theory calculations. Ni1 oligomerizes ethylene with high activity and selectivity for 1-butene production, while Ni2 showed even higher activity and selectivity under optimized reaction conditions. DFT calculations suggest that the higher activity of Ni2 is associated with its lowest unoccupied molecular orbital energy and highest natural charge at the Ni center.
APPLIED ORGANOMETALLIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Jinghua Xu, Ruifeng Wang, Lirong Zheng, Junguo Ma, Wenjun Yan, Xiaofeng Yang, Junying Wang, Xiong Su, Yanqiang Huang
Summary: The study investigated the nature of Ni active sites using Ni supported on alumina-silica as the catalyst, and found that Ni+ sites exhibit unprecedented activity in ethylene oligomerization, potentially directly participating in the formation of active sites.
CATALYSIS SCIENCE & TECHNOLOGY
(2021)
Article
Chemistry, Physical
Yue Cao, Yong Wu, Yuanteng Zhang, Jing Zhou, Wei Xiao, Dong Gu
Summary: Mesoporous cobalt oxide as a catalyst shows excellent performance in the synthesis of N-heterocycles, with high turnover numbers and easy recyclability for at least six times. Comparative studies reveal that the high surface area of the catalyst plays a crucial role in catalytic reactivity.
Article
Polymer Science
Hongwei Peng, Mingjun Ji, Jiaxing Li, Shuo Shen, Wanjuan Wang, Mengyu Chen, Guoshan He, Lihua Guo
Summary: Cycloalkyls were introduced into the pyridine-imine catalytic system to design a series of novel ligands and complexes for ethylene oligomerization. The nickel(II) complexes with cycloalkyl substituent exhibited high oligomerization activity and produced ethylene oligomers with low to moderate branching density. The palladium(II) complexes showed moderate oligomerization activity and yielded high branching density oligomers. Furthermore, the catalysts with flexible cycloalkyl substituents showed higher activity and generated oligomers with higher branching density compared to the catalyst with rigid phenyl substituent.
POLYMER INTERNATIONAL
(2023)
Article
Agricultural Engineering
Matthias Betz, Constantin Fuchs, Thomas A. Zevaco, Ulrich Arnold, Jorg Sauer
Summary: In the field of gasoline synthesis from renewable resources, highly integrated procedures are crucial for efficient and sustainable production. Ethylene oligomerization can produce gasoline-type hydrocarbons. Temperature and pressure significantly affect the selectivity and intramolecular branching. The catalyst showed stable performance under the tested conditions.
BIOMASS & BIOENERGY
(2022)
Article
Chemistry, Multidisciplinary
Florent Dubray, Vladimir Paunovic, Marco Ranocchiari, Jeroen A. van Bokhoven
Summary: This study investigates the oligomerization of pentene and hexene mixtures using an acidic mesoporous Al-SBA-15 catalyst. The results show that the catalyst exhibits high selectivity to jet-fuel range products (>98%) at low-to-moderate conversions (<50%). Higher conversions result in lower selectivities. It is also found that adjusting the conversion is the primary way to control the selectivity of the catalyst.
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Zhanshan Ma, Mengli Xu, Ningning Zhu, Chen Tan, Changle Chen
Summary: Heterogenization can improve the thermal stability and product morphology control of olefin polymerization catalysts, which are important parameters for industrial polyethylene production. In this study, alpha-diimine nickel catalysts with -OH or -ONa anchoring groups were designed and prepared to enable facile heterogenization on silica. The heterogeneous catalysts exhibited enhanced thermal stabilities and high catalytic activity, resulting in improvements in polymer morphology control, catalytic activity, and polyethylene molecular weight.
CHINESE JOURNAL OF CHEMISTRY
(2023)
Article
Energy & Fuels
Mingjie Liao, Xin Ning, Junwen Chen, Jiajun Zheng, Wenlin Li, Ruifeng Li
Summary: The synthesized mesoporous ZSM-5 zeolites showed better stability and higher initial activity in 1-hexene oligomerization compared to common ZSM-5 zeolite. The catalytic activity was closely related to the number and distribution of acid sites, with fewer and moderate strength of Bronsted acid sites inhibiting cracking and coke formation.
Article
Chemistry, Physical
Lin-Yan Bao, Rong-Wan Gao, Shuang Wang, Run-Han Li, Bo Zhu, Zhong-Min Su, Wei Guan
Summary: Photoredox/transition-metal dual catalysis is an efficient method for constructing C-N bonds. However, low recovery, low utilization rate, and high cost have hindered its application and development. By utilizing zinc powder, the oxidation state of nickel was successfully regulated, achieving a catalytic cycle without light.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
E. A. Jaseer, Nestor Garcia, Samir Barman, Mohamed Elanany, Motaz Khawaji, Hassan Alasiri, Niladri Maity
Summary: Phosphinite based ligands were evaluated for the first time in chromium catalyzed ethylene oligomerization, promoting the production of olefin products with a carbon number ranging from C6-C14. The highest productivity achieved was 12517 g/gCr.h.
Article
Multidisciplinary Sciences
Maximilian Baur, Fei Lin, Tobias O. Morgen, Lukas Odenwald, Stefan Mecking
Summary: By introducing reactive polar groups into polyethylene chains, phosphinophenolate-coordinated nickel complexes can facilitate the copolymerization of ethylene with carbon monoxide to create a new type of polymer with photodegradability. This material retains desirable material properties and exhibits environmental friendliness.
Article
Engineering, Chemical
Radu Dorin Andrei, Elena Borodina, Delphine Minoux, Nikolai Nesterenko, Jean-Pierre Dath, Claudia Cammarano, Vasile Hulea
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2020)
Article
Engineering, Chemical
Remi Beucher, Claudia Cammarano, Enrique Rodriguez-Castellon, Vasile Hulea
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2020)
Article
Chemistry, Organic
Laura Vaugon, Annie Finiels, Thomas Cacciaguerra, Vasile Hulea, Anne Galarneau, Cindy Aquino, Jean-Pierre Dath, Delphine Minoux, Corine Gerardin, Francois Fajula
PETROLEUM CHEMISTRY
(2020)
Article
Chemistry, Physical
Remi Beucher, Claudia Cammarano, Enrique Rodriguez-Castellon, Vasile Hulea
CATALYSIS COMMUNICATIONS
(2020)
Article
Materials Science, Multidisciplinary
Brindusa Dragoi, Cristina Mariana Uritu, Laurentiu Agrigoroaie, Doina Lutic, Thomas Cacciaguerra, Vasile Hulea, Eugen Carasevici
Summary: Manganese-based 2D nanoparticles with increased longitudinal relaxivity were synthesized through co-precipitation at low suprasaturation, showing excellent physico-chemical characteristics. The obtained relaxivity on a 1.0 Tesla apparatus at pH = 7.4 is significantly improved compared to other similar materials containing manganese.
Article
Chemistry, Applied
Atheer Al Khudhair, Karim Bouchmella, Radu Dorin Andrei, Ahmad Mehdi, P. Hubert Mutin, Vasile Hulea
Summary: The mixed oxide catalysts of SiO2-Al2O3-NiO with different Si/Al ratio and Ni content were prepared and evaluated in ethylene oligomerization. The study found that Si/Al ratio influenced the materials' texture and acidity, and samples with high Al content exhibited excellent performances. The catalysts compared well with model catalysts prepared by time-consuming multistep procedures from expensive ordered mesoporous silica supports.
MICROPOROUS AND MESOPOROUS MATERIALS
(2021)
Review
Chemistry, Physical
Vasile Hulea, Emil Dumitriu, Francois Fajula
Summary: This review discusses the importance of mild catalytic oxidation of thioethers and thiophenes, as well as the green synthesis principles using hydrogen peroxide as the oxidant and Me-containing porous materials as the best catalysts. It also addresses the catalytic active species generated in the presence of H2O2 and the probable oxidation mechanisms, as well as the role of solvents in the sulfoxidation process.
Article
Energy & Fuels
Chao Sun, Katarzyna Swirk Da Costa, Ye Wang, Li Li, Marco Fabbiani, Vasile Hulea, Magnus Ronning, Changwei Hu, Patrick Da Costa
Summary: Promoted Ni/Y/SBA-16 catalysts exhibited enhanced catalytic performance in CO2 methanation, with the catalyst promoted with 10 wt% Y showing the best activity. The improved performance was attributed to increased reducibility of nickel species, higher surface oxygen species, and the presence of moderate basic sites caused by yttrium promotion.
Article
Chemistry, Multidisciplinary
Remi Beucher, Vasile Hulea, Claudia Cammarano
Summary: A kinetic study of ethylene oligomerization on mesoporous 2 wt% Ni-AlKIT-6 was conducted in a fixed bed flow reactor. The main products identified were n-butenes and hexenes. The proposed Cossee-Arlman coordination-insertion mechanism explained the formation of these primary products. An activation energy and global kinetic order were determined, suggesting that ethylene insertion into the metal-alkyl bond is the kinetically limiting step.
REACTION CHEMISTRY & ENGINEERING
(2021)
Article
Chemistry, Multidisciplinary
Lucie Desmurs, Anne Galarneau, Claudia Cammarano, Vasile Hulea, Cyril Vaulot, Habiba Nouali, Benedicte Lebeau, T. Jean Daou, Carla Vieira Soares, Guillaume Maurin, Maciej Haranczyk, Isabelle Batonneau-Gener, Alexander Sachse
Summary: This paper describes specific corrections of the t-Plot method for different types of zeolite materials, allowing for more accurate evaluation of the surface properties of mesoporous zeolites. The corrected method is applied to characterize a variety of mesoporous zeolites.
Article
Nanoscience & Nanotechnology
Asma Fatnassi, Claudia Cammarano, Erwan Oliviero, Vasile Hulea, Nicolas Brun
Summary: In this study, a one-pot hydrothermal route for the atom-economical biosynthesis of C-aerogel-supported noble-metal nanoparticles was reported. By using renewable sugar derived from hemicellulose and natural phenol produced by brown algae as precursors, Pt/C and Ru/C nanocomposites with tunable properties were successfully prepared.
ACS APPLIED NANO MATERIALS
(2022)
Article
Chemistry, Physical
Lucie Desmurs, Claudia Cammarano, Gaetan Ramona, Robin Gaumard, Tzonka Mineva, Alexander Sachse, Jean-Dominique Comparot, Thomas Cacciaguerra, Didier Cot, Olinda Gimello, Anne Galarneau, Vasile Hulea
Summary: This study prepared mesoporous ZSM-5 catalysts using a 2-step micelle-templating procedure and varying the NaOH/Si synthesis ratio. The catalysts obtained showed different textural and acidic properties, with reduced acidity but higher mesopore volume. By testing two reactions, the best compromise was found for micro-/mesoporous ZSM-5 catalysts prepared with the ratio 0.38, which showed good accessibility for bulky molecules and specificity for Bronsted acid sites.
Review
Chemistry, Physical
Abdelilah Bayout, Claudia Cammarano, Izabel Medeiros Costa, Gleb Veryasov, Vasile Hulea
Summary: Methyl mercaptan is a useful molecule with various applications in industry. The largest segment of production uses methanol thiolation with tungsten-alumina catalysts, but alternative methods such as using syngas or catalytic hydrogenation have also been investigated. This comprehensive overview focuses on the production methods, their capabilities, and the role of catalysts used.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Review
Chemistry, Multidisciplinary
Vasile Hulea
Summary: This review focuses on the application of zeolite catalysts in isobutene reactions, including Prins condensation, isobutene dimerization, isobutene etherification, isobutene amination, and phenol tert-butylation. The mechanisms of these reactions, the role of zeolite catalysts, and the influence of topology/active sites on product selectivity are explored.
COMPTES RENDUS CHIMIE
(2022)
Article
Nanoscience & Nanotechnology
Brindusa Dragoi, Cristina Mariana Uritu, Laurentiu Agrigoroaie, Doina Lutic, Vasile Hulea, Georgeta Postole, Adina Coroaba, Eugen Carasevici
Summary: Nanotheranostic materials containing manganese as a contrast agent for MRI and fluorouracil as an anticancer drug were prepared with two synthetic approaches. The materials were extensively characterized, showing high-quality 2D structures with high relaxivities for MRI imaging.
ACS APPLIED NANO MATERIALS
(2021)
