Article
Polymer Science
Lixin Cao, Zhengguo Cai, Mingyuan Li
Summary: A series of nickel complexes with substituted phenylphosphine ligands were synthesized and characterized. These complexes showed high activity and thermal stability in norbornene polymerization. They could also copolymerize norbornene and methyl acrylate to produce functionalized cyclic olefin copolymer, and copolymerize ethylene and methyl acrylate to produce polar functionalized polyethylene.
Article
Chemistry, Physical
Yuanrui Wang, Xiao-Feng Wu
Summary: A palladium-catalyzed redox-neutral dicarbonylation of terminal alkynes has been developed, using hydroxylamine as both a nucleophile and a potential oxidant. Maleimides were synthesized in moderate yields under relatively mild conditions without the addition of equivalent oxidants. This reaction involves Pd-H addition to the alkyne and the role of hydroxylamine ester intermediate as an internal oxidant via nucleophilic attack.
JOURNAL OF CATALYSIS
(2023)
Article
Polymer Science
Kosuke Isaji, Shin-ichi Matsuoka, Masato Suzuki
Summary: A new copolymer of NB with exo-NBL was successfully synthesized using Pd catalytic systems, leading to a polymer with improved solubility in chlorinated solvents and high thermal stability. This copolymer showed a random sequence and enhanced physical properties compared to poly(NB).
JOURNAL OF POLYMER SCIENCE
(2021)
Article
Chemistry, Multidisciplinary
Xin Liu, Yun Zhou, Xiaotian Qi, Renhe Li, Peng Liu, Guangbin Dong
Summary: A site- and regioselective vicinal di-carbo-functionalization of indoles has been realized by the palladium/norbornene (Pd/NBE) cooperative catalysis. The C1-substituted NBE plays a key role in promoting the turnover-limiting oxidative addition step.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Applied
Dmitry S. Suslov, Zorikto D. Abramov, Ilya A. Babenko, Viktor A. Bezborodov, Tatyana N. Borodina, Mikhail V. Bykov, Marina V. Pakhomova, Vladimir I. Smirnov, Anastasia V. Suchkova, Gennadii V. Ratovskii, Igor A. Ushakov, Alexey I. Vilms
Summary: The Pd(II) complexes with thioether ligands exhibited high catalytic activity in the addition polymerization, showing differences in structural features in both solid state and solution.
APPLIED ORGANOMETALLIC CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Dmitry S. Belov, Logesh Mathivathanan, Melanie J. Beazley, William Blake Martin, Konstantin V. Bukhryakov
Summary: The study explores the capability of an iron-based catalyst in performing ring-opening metathesis polymerization of olefins, demonstrating that the use of in situ prepared heteroleptic iron catalysts significantly enhances polymerization rate and selectivity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Ah Rim Jeong, Saira Nayab, Eunhee Kim, Hyeonuk Yeo, Hyosun Lee
Summary: A series of Pd(II) complexes bearing N,N-bidentate aminomethylpyridine and aminomethylquinoline derivatives were synthesized and characterized. The complexes showed significant catalytic activities towards the addition polymerization of norbornene and methyl methacrylate in the presence of modified methylaluminoxane (MMAO). Complex 3 with quinoline/piperidine functionalities exhibited the highest catalytic activity and produced high molecular weight polymers.
JOURNAL OF MOLECULAR STRUCTURE
(2022)
Article
Chemistry, Physical
Wilhelm H. le Roux, Megan Matthews, Albena Lederer, Albert J. van Reenen, Rehana Malgas-Enus
Summary: Ten novel Schiff-base functionalized nickel nano-systems were synthesized and evaluated as catalysts in polymerization reactions. The nanoparticles exhibited good stability and activity, demonstrating diverse functionalities in polymerization processes.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Multidisciplinary
Hongyu Guo, Sheng Zhang, Yang Li, Xiaoqiang Yu, Xiujuan Feng, Yoshinori Yamamoto, Ming Bao
Summary: A palladium-catalyzed tail-to-tail reductive dimerization reaction of terminal alkynes is reported for the first time, leading to the efficient transformation of aromatic and aliphatic alkynes into 2,3-dibranched butadienes. The control of reaction solution acidity, achieved by a combination of pivalic acid and para-toluenesulfonic acid, is crucial for the selective tail-to-tail reductive dimerization reaction, which is proposed to proceed via a cationic alkenyl palladium intermediate under acidic conditions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Polymer Science
Wenbing Wang, Min Chen, Wenmin Pang, Yougui Li, Chen Zou, Changle Chen
Summary: Investigated two groups of norbornene comonomers: one provides additional active sites for sulfur vulcanization and the other can alter the non-polar nature of polyolefin materials. Palladium-catalyzed terpolymerization of ethylene with these comonomers yields polar-functionalized polyolefin elastomers with high molecular weight and comonomer content, possessing excellent mechanical and elastic properties.
Article
Multidisciplinary Sciences
Menghe Xu, Changle Chen
Summary: The article explores a method utilizing 5,6-disubstituted norbornenes as comonomers to address challenges in the copolymerization of olefins with polar comonomers using catalysts. The use of phosphine-sulfonate palladium catalysts enables high polymerization activity, copolymer molecular weight, and comonomer incorporation, resulting in polar-functionalized polyolefins.
Article
Chemistry, Applied
Hayeon Kwak, Eunsu Kang, Jae Yeong Song, Geunhee Kang, Jung Min Joo
Summary: The development of modular approaches for heteroaromatic cores and substituents is crucial for drug candidates and organic functional materials. A new strategy involving the cyclization of heteroarenes tethered with alkynes through a norbornene bridge was developed. The Pd catalytic system transformed a variety of five-membered heteroarenes to the corresponding benzofused products, demonstrating its versatility in the annulation of (hetero)aromatic rings.
ADVANCED SYNTHESIS & CATALYSIS
(2021)
Article
Chemistry, Organic
Ashok Donthoju, Anandarao Munakala, Sushma Ellandula, Rambabu Chegondi
Summary: In this study, we have reported a palladium(0)-catalyzed decarboxylative oxa-Michael addition/remote alpha-allylation/1,3-migration reaction with high yields. The reaction is triggered by a base-mediated retro-Michael ring-opening reaction and subsequent syn-selective oxa-Michael addition.
JOURNAL OF ORGANIC CHEMISTRY
(2022)
Article
Polymer Science
Linfeng Wang, Shuqi Dong, Hui Tian, Guangbi Gong, Baoli Wang, Chunji Wu, Dongmei Cui
Summary: We report the terpolymerization of ethylene, norbornene, and dicyclopentadiene using fused-heterocyclic and pyridyl-modified cyclopentadienyl scandium complexes. The resulting E/NB/DCPD terpolymers exhibited adjustable structures and high glass-transition temperature. The incorporation of cycloolefin units into the terpolymers was observed and attributed to the use of two kinds of cycloolefins and efficient scandium catalysts.
Article
Chemistry, Physical
Dilip K. Pandey, Eugene Khaskin, Shrinwantu Pal, Robert R. Fayzullin, Julia R. Khusnutdinova
Summary: We describe an efficient semihydrogenation of terminal alkynes using a modified tetramethylated PNP pincer Fe hydride complex. The modified complex shows different reactivity compared to a classical PNP Fe hydride complex with CH2 arms, which predominantly catalyzes terminal alkyne dimerization even in the presence of H-2. The modified PNP ligand allows for selective alkene formation, eliminating dimerization side products and minimizing overreduction.
Article
Multidisciplinary Sciences
Chen Zou, Guifu Si, Changle Chen
Summary: The authors present an ionic anchoring support strategy that allows the heterogenization of homogeneous metal complexes on solid supports. This strategy is highly versatile and enables strong catalyst-support interactions while tolerating various polar functional groups. The supported catalysts showed improved polymerization properties and higher comonomer incorporation compared to their unsupported counterparts.
NATURE COMMUNICATIONS
(2022)
Article
Polymer Science
Amir Mohammad Mansouri, Mehrsa Emami, Saleh Yousefi, Changle Chen, Mahdi Hashemzadeh Gargari, Ahad Hanifpour, Naeimeh Bahri-Laleh
Summary: This study quantified the microstructural, flow, and mechanical properties of two commercially available HDPE samples with different particle sizes. The results showed that the film grade sample had larger particle sizes and better mechanical properties compared to the blow molding sample.
JOURNAL OF APPLIED POLYMER SCIENCE
(2022)
Article
Chemistry, Multidisciplinary
Changwen Hong, Zihao Wang, Hui Jiang, Guifu Si, Maoping Song, Changle Chen
Summary: Brookhart-type α-diimine nickel and palladium catalysts have been extensively studied, but their heterogenization has received less attention. In this study, a trifluoroborate potassium substituent was introduced on an α-diimine framework. The ionic nature of trifluoroborate potassium strengthened the interaction between the α-diimine nickel complex and SiO2 support, while its electron-donating property enhanced the catalyst stability and polyethylene molecular weight.
CHINESE CHEMICAL LETTERS
(2023)
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
Chemistry, Physical
Shi-Yu Chen, Yu-Hang Song, Shuang Jiao, Chen Zou, Shi-Huan Li, Changle Chen, Xiao-Bing Lu, Ye Liu
Summary: Polyethylenes are widely used synthetic polymers, and introducing functional groups into polyethylene backbone can improve environmental persistence and compatibility with other materials. However, this process is hindered by the formation of alternating polyketones. By reducing the carbonyl density in polyketones, their properties become closer to polyethylene. In this study, Ni and Pd-coordinated cationic catalysts were used for nonalternating carbonylative copolymerization of ethylene, resulting in car-bonyl functionalized polyethylenes with similar properties to commercial high-density polyethylene.
JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Multidisciplinary
Jie Li, Dan Peng, Chen Tan, Changle Chen
Summary: In this contribution, an outer-shell self-supporting strategy was designed to heterogenize nickel catalysts on different fillers via precipitation homopolymerization of ionic cluster type polar monomer. These catalysts demonstrated high activity, good product morphology control, and stable performances in ethylene polymerization and copolymerization. Moreover, various polyolefin composites with great mechanical and customized properties can be efficiently synthesized.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Inorganic & Nuclear
Yan-Bing Wang, Chenlong Nan, Weize Zhuo, Chen Zou, Hui Jiang, Xin-Qi Hao, Changle Chen, Mao-Ping Song
Summary: The introduction of O-donor groups on amine-imine ligands leads to the synthesis of a series of nickel complexes, which exhibit high catalytic activities and produce polyethylene elastomers with high molecular weight. Moreover, these nickel complexes can also catalyze the copolymerization of ethylene with various functional monomers to prepare functionalized polyolefins.
INORGANIC CHEMISTRY
(2023)
Article
Polymer Science
Somayyeh Sadat Afi Kheljani, Khadijeh Didehban, Mohammad Atai, Changle Chen, Naeimeh Bahri-Laleh
Summary: In this research, the functionalization of easily available polyalphaolefin (PAO) based resins was achieved through copolymerization and further modification. The microstructure of the synthesized and modified resins was analyzed using various analytical methods. The resulting macromer showed a hydrophilic nature and had potential applications in tissue engineering.
JOURNAL OF POLYMER RESEARCH
(2023)
Article
Polymer Science
Dan Peng, Menghe Xu, Chen Tan, Changle Chen
Summary: In this study, an emulsion polymerization strategy was used to heterogenize imino-based nickel olefin polymerization catalysts on solid supports. Polymeric microspheres were prepared through emulsion copolymerization, and the resulting heterogeneous nickel catalysts exhibited excellent properties in ethylene polymerization and copolymerization. The catalytic properties could be controlled by adjusting the comonomer type, composition, and particle size. This strategy allowed for product morphology control, avoided reactor fouling, and generated polyethylene products with minimal inorganic contamination. Furthermore, the introduction of polymer microspheres improved the mechanical and surface properties of polyolefin products.
Article
Polymer Science
Menghe Xu, Ao Chen, Wu Li, Yougui Li, Chen Zou, Changle Chen
Summary: Introducing polar biomass groups into polyolefins improves their nonpolar nature and aligns with sustainable development. Researchers have developed an efficient method to produce polar functionalized polyolefins with high biomass content. By utilizing phosphine-sulfonate palladium-catalyzed copolymerization reactions, bioresourced comonomers with oleyl and cinnamyl groups are inserted into the polyolefins.
Article
Chemistry, Physical
Jie Xu, Changle Chen, Xiangkai Kong
Summary: Controlled alloying, structure design, phase exploration, and carbon support modulation strategies are used for efficient Ru-based catalyst synthesis. A stepped annealing approach is employed to create Ru active sites, where Ru nanocrystals are in-situ formed on CuO surface and strong interaction at the interface is generated. The resultant Ru-CuO-SA catalyst exhibits high overpotential, low Tafel slope, and high turnover frequency, surpassing most reported materials. The creation of Ru-O-Cu bonds enhances surface oxophilicity and provides moderate hydrogen binding, resulting in improved hydrogen production efficiency.
Review
Chemistry, Multidisciplinary
Chen Tan, Min Chen, Changle Chen
Summary: Transition metal-catalyzed olefin-polar monomer copolymerization has the potential to synthesize polar group-functionalized polyolefin materials. However, the traditional trial-and-error approach is challenging and time-consuming. Recent 'catalyst + X' strategies have emerged, which utilize the interactions between the catalyst and other components in the copolymerization system to influence the reaction and resulting material properties. This review summarizes selected examples of these strategies and discusses future perspectives.
TRENDS IN CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Chen Zou, Chen Tan, Changle Chen
Summary: Polyolefins are commonly used synthetic polymers, but their limited compatibility with polar materials has hindered their application in certain fields. Transition-metal-catalyzed copolymerization of olefin and polar functionalized monomers allows for the synthesis of polar-functionalized polyolefin materials with improved properties. Heterogenization strategies for the synthesis of high-performance heterogeneous nickel catalysts have been developed, offering better control over product morphology and improved polymerization processes.
ACCOUNTS OF MATERIALS RESEARCH
(2023)
Article
Multidisciplinary Sciences
Chen Zou, Quan Wang, Guifu Si, Changle Chen
Summary: Polar bimodal polyethylene is demonstrated as a potential solution to the trade-off between catalytic activity and polymer molecular weight caused by polar groups in catalysts. Three synthetic routes are investigated to achieve high miscibility between the polar and non-polar fractions, with the co-anchoring strategy being the most effective. This produces polyolefin materials with excellent properties for various applications.
NATURE COMMUNICATIONS
(2023)
Article
Polymer Science
Daohong Liao, Wenmin Pang, Muhammad Sohail Bashir, Changle Chen
Summary: Tacticity plays a significant role in the characteristics of synthetic polymers. This study presents a tubular reactor strategy for continuous flow polymerization of isobutyl vinyl ether (IBVE), resulting in highly stereoselective poly(IBVE). The obtained poly(IBVE) product demonstrates technical advantages for potential industrial applications.