Article
Multidisciplinary Sciences
Houqian Li, Jiayang Wu, Zhen Jiang, Jiaze Ma, Victor M. Zavala, Clark R. Landis, Manos Mavrikakis, George W. Huber
Summary: Waste plastics can be used as a feedstock for the production of renewable chemicals. By pyrolysis, waste plastics can be converted into pyrolysis oils containing high concentrations of olefins. These olefins can be used to produce aldehydes through hydroformylation, and further transformed into valuable oxygenated chemicals through various catalytic processes. The use of this route could significantly reduce greenhouse gas emissions compared to traditional petroleum-based production methods.
Review
Chemistry, Inorganic & Nuclear
Vincenzo Balzani, Paola Ceroni, Alberto Credi, Margherita Venturi
Summary: [Ru(bpy)(3)](2+) and its related compounds are a unique family of clever molecules that can process optical and electrical signals, and perform a variety of interesting functions as components of chemical species.
COORDINATION CHEMISTRY REVIEWS
(2021)
Review
Energy & Fuels
Mrityunjay K. Sharma, Ryan L. Hartman
Summary: Polyolefins are the most produced plastics in the world, and the properties of polyolefins are strongly affected by reactor conditions. Microfluidics combined with machine-learning algorithms can play a significant role in designing and optimizing polymer properties.
Article
Chemistry, Multidisciplinary
Daniel Hugenbusch, Marc Lehr, Jan-Simon von Glasenapp, Anna J. McConnell, Rainer Herges
Summary: We report the photo-switching properties of two regioisomeric diazocine ligands. The self-assembly of these ligands with Co-II ions was studied, and reversible transformation between different ligand configurations and Co-II complexes was achieved through light-controlled switching.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Esther Nieland, Jona Voss, Andreas Mix, Bernd M. Schmidt
Summary: This study demonstrates the use of visible light to shift dynamic covalent imine assemblies out of equilibrium. A fluorinated azobenzene building block was combined with different amines to create a library of imine macrocycles. The chiral amine provides access to a rich network of macrocycles that undergo isomerisation and interconversion between different species.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Review
Chemistry, Inorganic & Nuclear
Federico Nicoli, Erica Paltrinieri, Marina Tranfic Bakic, Massimo Baroncini, Serena Silvi, Alberto Credi
Summary: Living systems rely on ions and molecules for information processing and motion control. Artificial mimics of biomolecular systems have been developed, and their combination can produce logic-controlled nanomachines with great potential for applications. These systems may lead to the development of 'molecular robots' capable of executing specific functions based on environmental stimuli.
COORDINATION CHEMISTRY REVIEWS
(2021)
Article
Chemistry, Applied
Hongwei Peng, Shuaikang Li, Gen Li, Shengyu Dai, Mingjun Ji, Zhe Liu, Lihua Guo
Summary: The addition of bulky rotation-restricted substituents into iminopyridyl Ni (II) and Pd (II) catalysts was shown to effectively retard chain transfer, resulting in high molecular weight polyethylene or ethylene-MA copolymers with high MA incorporation ratio. Systematic studies on the (co)polymerization behavior as a function of rotation-restricted substituent variations led to the successful synthesis of various molecular weight polyethylene and ethylene-MA copolymer products.
APPLIED ORGANOMETALLIC CHEMISTRY
(2021)
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
Chemistry, Multidisciplinary
Andre Seco, Shilin Yu, Arnaud Tron, Nathan D. McClenaghan, Fernando Pina, A. Jorge Parola, Nuno Basilio
Summary: A linear double pyridinium-terminated thread with a central chalcone moiety provides two independent binding sites for cucurbit[7]uril macrocycles in water. The association leads to [2] and [3] pseudorotaxanes, which are pH and photosensitive, with enhanced association upon switching to the cationic flavylium form. Threading the flavylium moiety into CB7 results in a significant increase in fluorescence quantum yield.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Hao Hu, Hua Wang, Yuchong Yang, Jiang-Fei Xu, Xi Zhang
Summary: In this study, a cationic porphyrin derivative TMPyP was developed that could be used for specific bacteria-responsive antimicrobial treatment through adaptable photodynamic/photothermal therapy processes. The results showed that TMPyP exhibited strong antimicrobial activity (>99%) through photothermal therapy in hypoxic environments where facultative anaerobes with a strong reducing ability, such as E. coli and S. typhimurium, could reduce TMPyP to phlorin. In aerobic environments with aerobic bacteria, TMPyP functioned as a typical photosensitizer that effectively killed bacteria (>99.9%) through photodynamic therapy. The biocompatibility of TMPyP was significantly improved by forming a host-guest complex with cucurbit[7]uril. This bacteria-responsive porphyrin demonstrates specificity and adaptability in antimicrobial treatment and holds potential in non-invasive treatments of bacterial infections.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Polymer Science
Duarte M. Cecilio, Auguste Fernandes, Joao Paulo Lourenco, Timothy F. L. McKenna, M. Rosario Ribeiro
Summary: This study developed an innovative methodology for preparing high-performance polyolefin-based materials, combining a unique dendrimeric silica carrier, a straightforward in situ supporting procedure, and in situ ethylene polymerization technique. By applying an in situ supporting procedure, highly active catalysts were obtained, simplifying the experimental set-up and potentially leading to significant cost savings in the production of HDPE nanocomposite materials with tunable properties.
Review
Chemistry, Inorganic & Nuclear
Joakim Andreasson, Uwe Pischel
Summary: This review discusses the use of light in addressing stimuli-responsive molecular and supramolecular systems, focusing on molecular photoswitches. Light provides advantages in terms of spatiotemporal control and remote triggering, allowing for precise design of excited state processes for desired logic operations or functions. Photons as traceless reagents enable the recycling and reconfiguration of devices, merging photoswitching with information processing.
COORDINATION CHEMISTRY REVIEWS
(2021)
Article
Chemistry, Multidisciplinary
Berengere Aubry, Remi Canterel, Muriel Lansalot, Elodie Bourgeat-Lami, Aissam Airoudj, Bernadette Graff, Celine Dietlin, Fabrice Morlet-Savary, Jan Blahut, Ladislav Benda, Guido Pintacuda, Emmanuel Lacote, Jacques Lalevee
Summary: The utilization of N-heterocyclic carbene-borane complexes in a borane-(meth)acrylate click reaction has shown promising results in developing polymers with improved properties for 3D printing fuels. The increased network density and faster polymerization kinetics due to the higher bond number of boranes relative to thiols contribute to enhanced mechanical properties and reduced solvent swelling in the materials. Solid-state NMR, DMA, and AFM techniques confirm the significant role of boron centers in influencing the network properties of the materials.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Sylvain Sudan, Farzaneh Fadaei-Tirani, Rosario Scopelliti, Kristina E. Ebbert, Guido H. Clever, Kay Severin
Summary: Thirteen palladium-ligand assemblies with different structures and topologies were studied for their ability to bind lithium ions. It was found that the addition of LiBF4 caused a significant structural rearrangement in one case, converting a dinuclear [Pd2L4](4+) complex into a low-symmetry [Pd4L8](8+) assembly with two binding pockets for solvated LiBF4 ion pairs. This rearrangement was only induced by Li+, indicating highly specific host-guest interactions. Structural analysis revealed that the [Pd4L8](8+) receptor had a compact structure with multiple intramolecular interactions, similar to natural and synthetic foldamers.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Polymer Science
Yangke Xiao, Pingwei Liu, Wen-Jun Wang, Bo-Geng Li
Summary: This study demonstrates a method for preparing polyolefin elastomers with tunable dynamic chemical cross-linking, compatible with industrial production, showing high mechanical performance and thermal stability. After multiple reprocessing, the elastomers maintain high performance, indicating the potential for developing high-performance polyolefins with good reprocessability and recyclability in the future.
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.