Article
Chemistry, Inorganic & Nuclear
Michal Terlecki, Iwona Justyniak, Michal K. Leszczynski, Piotr Bernatowicz, Janusz Lewinski
Summary: Organozinc amidinates, specifically alkylzinc complexes supported by N,N-bidentate ligands, have been extensively studied in various fields. However, the corresponding organozinc amidinates are still poorly explored. This study aims to investigate the factors influencing the structure and stability of alkylzinc amidinates by modifying the Zn center's secondary coordination sphere. Through synthesis and characterization techniques, it was found that the [RZnL](x)-type amidinate moieties are unstable and tend to undergo ligand scrambling, forming more thermodynamically stable non-stoichiometric complexes.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Multidisciplinary
Shaowu Du, Meiyan Cui, Zhangzhen He
Summary: A new pentanuclear {Co-5} cluster motif with a D-3h oblate trigonal bipyramidal geometry was discovered, forming a unique capped breathing kagome lattice. Magnetic results indicated paramagnetism at 2 K, with the disappearance of two-thirds of the spin moment at low temperatures and the appearance of a 1/5 magnetization plateau.
CHEMICAL COMMUNICATIONS
(2021)
Article
Chemistry, Multidisciplinary
Huiqing Yuan, Jiehao Du, Mei Ming, Ya Chen, Long Jiang, Zhiji Han
Summary: The study introduces a multimetallic Fe2Na3 purpurin complex for CO2 reduction in DMF under visible-light irradiation, achieving high selectivity and turnover. The mechanism involves reductions and protonations of the complex to generate active photocatalysts for CO2 reduction.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Inorganic & Nuclear
Gabriele Manca, Fabrizia Fabrizi de Biani, Maddalena Corsini, Cristiana Cesari, Cristina Femoni, Maria Carmela Iapalucci, Stefano Zacchini, Andrea Ienco
Summary: This article provides a detailed analysis of the electronic structure of the pentanuclear bow tie Au/Fe carbonyl cluster [Au{eta(2)-Fe-2(CO)(8)}(2)](-) and questions the traditional assignment of gold in the +3 oxidation state.
INORGANIC CHEMISTRY
(2022)
Review
Chemistry, Multidisciplinary
Biswanath Das, Ahibur Rahaman, Andrey Shatskiy, Oscar Verho, Markus D. Karkas, Bjorn Akermark
Summary: Research efforts have been focused on designing efficient catalysts for water oxidation, with a particular interest in ruthenium-based catalysts due to their robust nature and high activity. Strategic modifications of ligand structures to enable proton-coupled electron transfer (PCET) and atom proton transfer (APT) play a central role in improving the catalysts' performance for O-O bond formation during water oxidation. Introduction of carboxylate groups in the ligands has been shown to improve stability, prevent metal leaching, and enhance proton donor/acceptor properties, ultimately leading to improved efficiency and reduced overpotential in the water oxidation reaction.
ACCOUNTS OF CHEMICAL RESEARCH
(2021)
Article
Chemistry, Inorganic & Nuclear
Sokratis T. Tsantis, Panagiota Danelli, Demetrios Tzimopoulos, Catherine P. Raptopoulou, Vassilis Psycharis, Spyros P. Perlepes
Summary: The reaction system produces a pentanuclear cluster with the doubly deprotonated form of the gem-diol derivative, representing the first characterized Th-5(IV) complex. The structural analysis reveals it is a Kuratowski-type coordination compound.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Inorganic & Nuclear
Jian Tang, Liang Zhao
Summary: This study focuses on controlling the synthesis of chiral metal clusters by adjusting factors such as nuclearity number, metal-metal interaction, and spatial arrangement of metal atoms. The research found that the chiroptical response of the acquired metal clusters was mainly influenced by the geometrically twisted arrangement of metal atoms. The tetranuclear gold cluster compound with the shortest intermetallic interaction and the largest torsion angle showed the highest absorption anisotropy factor. The correlation between structural factors and the stability of chiral gold clusters was also evaluated.
INORGANIC CHEMISTRY
(2022)
Review
Chemistry, Inorganic & Nuclear
Nobuto Yoshinari, Takumi Konno
Summary: Organic polycarboxylates are important building units in supramolecular chemistry for constructing coordination and hydrogen-bonded frameworks. This review focuses on multifunctional metal-organic carboxylates (MOCs) with multiple noncoordinating carboxylate groups, which can be used as pre-prepared metalloligands for constructing metal-organic frameworks. The stability and diverse structures of MOCs make them promising candidates for various applications.
COORDINATION CHEMISTRY REVIEWS
(2023)
Article
Chemistry, Multidisciplinary
Chen Zeng, Qing-Dou Xu, Xiao-Lin Liu, Yu-Ying Yang, Sheng-Min Hu, Xin-Tao Wu, Tian-Lu Sheng
Summary: A series of trimetallic and pentanuclear compounds were synthesized and characterized. The investigation revealed the presence of specific metal-metal interactions in these compounds.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Inorganic & Nuclear
Vijay Gupta, Iwona Justyniak, Elzbieta Chwojnowska, Vadim Szejko, Janusz Lewinski
Summary: This study presents the synthesis and structural characterization of a zinc-magnesium benzoate framework, which forms stable Lewis acid-base adducts and exhibits high copolymerization activity at elevated temperatures.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Applied
Pauline Schiltz, Mengyu Gao, Corentin Ludwig, Corinne Gosmini
Summary: In this study, a direct method for preparing alkylzinc compounds from functionalized alkyl bromides using cobalt catalysis under mild conditions was reported. The reaction is stable under air and moisture conditions, making it an accessible procedure. Various functional groups on primary and secondary alkyl bromides, including esters, cyano, and halogens, were well-tolerated, resulting in high yields of the corresponding alkylzinc compounds. The alkylzinc derivatives were successfully applied in palladium-catalyzed Negishi cross-coupling with different functionalized aryl bromides, demonstrating the efficiency and robustness of the methodology.
ADVANCED SYNTHESIS & CATALYSIS
(2023)
Article
Chemistry, Inorganic & Nuclear
Ying Wang, Yan Ni Zhou, Yu Liang, Lin Cheng, Yu Fang
Summary: A novel three-dimensional copper-organic framework with high sensitivity and selectivity towards dysprosium ion (Dy3+) and luminescent quenching towards cyano compounds has been designed and synthesized, showing potential as a luminescent probe for various inorganic and organic compounds.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Organic
Marine Pinaud, Emilie Plantiveau, Eric Huet, Erwan Le Gall, Marc Presset
Summary: Mannich-type reactions involving alkylzinc reagents have been developed using different strategies. We found that simple heating allows the addition of these organometallic species to sulfonyl imines, giving Mannich products in moderate to excellent yields (14 examples, 30-99%). Interestingly, N-alkyl imines can also be used as suitable partners after activation as an acyliminium by acetyl chloride (12 examples, 49-86%) or, more originally, by TMSCl (14 examples, 26-87%). These methods are complementary, providing both N-protected secondary or tertiary amines and N-unprotected secondary amines in good yields, with improved eco-compatibility and under simple conditions.
EUROPEAN JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Jie Lin, Kaixin Chen, Jixin Wang, Jiawei Guo, Siheng Dai, Ying Hu, Jie Li
Summary: The construction of Csp(3)-Csp(3) bonds using alkylzinc reagents through Negishi-type reactions is highly important for the synthesis of pharmaceuticals and agrochemicals. However, the conventional alkylzinc halides have limitations in terms of reactivity and generality. In this study, we successfully prepared solid and salt-stabilized alkylzinc pivalates by OPiv-coordination, which exhibited enhanced stability and excellent reactivity in a cobalt-catalyzed difluoroalkylation-alkylation of dienoates, allowing for the selective installation of CF2- and Csp(3)-groups across double bonds.
Article
Chemistry, Multidisciplinary
Sayantan Ganguly, Pradip Bhunia, Julia Mayans, Ashutosh Ghosh
Summary: One new heterometallic nickel(II)-manganese(II) complex and two new copper(II)-manganese(II) complexes have been synthesized and structurally characterized. These complexes exhibit catecholase-like activity in the oxidation reaction and show antiferromagnetic exchange interactions.
NEW JOURNAL OF CHEMISTRY
(2022)
Article
Polymer Science
Georgina L. Gregory, Charlotte K. Williams
Summary: This study presents a closed-loop recyclable thermoplastic elastomer (TPEs) with well-controlled block polyester TPEs featuring regularly placed sodium/lithium carboxylate side chains. These TPEs show significantly higher tensile strengths, high elasticity, and elastic recovery compared to unfunctionalized analogues. The materials are prepared using controlled polymerizations and can be recycled without loss of mechanical properties.
Review
Chemistry, Multidisciplinary
Wilfred T. Diment, Wouter Lindeboom, Francesca Fiorentini, Arron C. Deacy, Charlotte K. Williams
Summary: The development of sustainable plastic materials using sustainable monomers and polymers that can be chemically recycled is a key goal of 21st century chemistry. However, designing efficient catalysts for these processes remains challenging due to issues such as low catalytic activities, high catalyst loading requirements, and the need for costly, toxic cocatalysts.
ACCOUNTS OF CHEMICAL RESEARCH
(2022)
Article
Chemistry, Multidisciplinary
Georgina L. Gregory, Gregory S. Sulley, Joost Kimpel, Matylda Lagodzinska, Lisa Hafele, Leticia Pena Carrodeguas, Charlotte K. Williams
Summary: This study reports well-defined reprocessable poly(ester-b-carbonate-b-ester) elastomers with impressive physical properties and degradability. The superior performance of these elastomers is attributed to the highly entangled soft segments, fully reversible strain-induced crystallization, and precisely placed Zn-II-carboxylates dynamically crosslinking the hard domains.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Georgina L. Gregory, Hui Gao, Boyang Liu, Xiangwen Gao, Gregory J. Rees, Mauro Pasta, Peter G. Bruce, Charlotte K. Williams
Summary: Polymers with specific properties can help overcome challenges in all-solid-state batteries, resulting in improved capacity retention.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Thomas M. McGuire, Arron C. Deacy, Antoine Buchard, Charlotte K. Williams
Summary: The study demonstrates the chemical recycling of aliphatic polycarbonates using a heterodinuclear [Mg(II)Co(II)] catalyst under solid-state conditions, showing high activity and selectivity. This approach is not only efficient but also allows for multiple reuses of the catalyst.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Kam C. Poon, Georgina L. Gregory, Gregory S. Sulley, Fernando Vidal, Charlotte K. Williams
Summary: Using CO2 to make polycarbonates through ROCOP reduces pollution in polymer manufacturing. Recent developments in catalysis allow for the copolymerization with biomass-derived monomers, but the resulting material properties are underinvestigated.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Bradley E. Cowie, Lisa Hafele, Andreas Phanopoulos, Said A. Said, Ja Kyung Lee, Anna Regoutz, Milo S. P. Shaffer, Charlotte K. Williams
Summary: This work demonstrates the use of organometallic routes for the synthesis of copper(0/I) nanoparticles and emphasizes the importance of ligand selection to achieve desired material compositions. By reacting an organo-copper precursor with hydrogen, air or hydrogen sulfide, Cu, Cu2O or Cu2S nanoparticles can be obtained. Sub-stoichiometric amounts of protonated ligands are used to avoid excess contamination, and ligand exchange reactions reveal different coordination tendencies for copper(0) nanoparticles compared to Cu2O and Cu2S. This study highlights the potential of organometallic methods for well-defined nanoparticles and underscores the significance of ligand chemistry.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Jamie T. T. Wilmore, Yuen Cheong Tse, Andrew Docker, Caspar Whitehead, Charlotte K. K. Williams, Paul D. D. Beer
Summary: A series of dynamic metalloporphyrin [2]rotaxane molecular shuttles were synthesized with high yield using active metal template synthetic methodology. The dynamic macrocycle translocation is controlled by an inter-component co-ordination interaction between the macrocycle pyridyl and axle Zn(II) metalloporphyrin. The shuttling behavior can be inhibited by a neutral Lewis base, but can be tuned through rotaxane demetallation or subsequent metallation.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Fernando Vidal, Sevven Smith, Charlotte K. Williams
Summary: Boron-functionalized polymers have wide applications in opto-electronics, biology, and medicine. However, methods to produce boron-functionalized and degradable polyesters are rare. This study presents a controlled ring-opening copolymerization method to produce boron-functionalized polyesters. The resulting polymers have adjustable structures, molecular weights, and boron functionalities. The boronic ester-functionalized polymers are amorphous and have high glass transition temperatures and good thermal stability. The utility of this method is demonstrated by synthesizing fluorescent spherical nanoparticles. This versatile technology provides a platform for future explorations of degradable and functional polymers.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Wouter Lindeboom, Arron C. Deacy, Andreas Phanopoulos, Antoine Buchard, Charlotte K. Williams
Summary: Carbon dioxide copolymerization is a promising strategy for CO2 utilization, but the success depends on improving the catalysis. However, the relationship between catalyst structure and performance is not straightforward, which limits the ability to predict and enhance both catalytic activity and selectivity. In this study, a simple measure of a catalyst ground-state parameter, metal reduction potential, is shown to directly correlate with both polymerization activity and selectivity. This method has been successfully applied to compare the performance of 6 new heterodinuclear Co(III)K(I) catalysts for CO2 copolymerization, providing valuable insights for future catalyst discovery.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Thomas M. McGuire, Antoine Buchard, Charlotte Williams
Summary: This study presents an efficient method for chemical recycling of waste Poly(L-lactic acid) (PLLA) using a commercial Sn(II) catalyst and nonvolatile commercial alcohol. The depolymerization of PLLA to yield pure L-lactide (L-LA) can be achieved at low temperatures, and the catalyst system shows outstanding activity and selectivity. Furthermore, the catalyst system can be recycled multiple times without loss of its catalytic productivity.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Francesca Fiorentini, Wilfred T. T. Diment, Arron C. C. Deacy, Ryan W. F. Kerr, Stephen Faulkner, Charlotte K. K. Williams
Summary: In this study, a series of heterodinuclear catalysts based on Co(III) combined with alkali and alkaline earth metals were evaluated for three different polymerization reactions. The results show that catalysts with lower Lewis acidity exhibit higher reaction rates and selectivity. These structure-performance correlations apply across different polymerization reactions and provide valuable insights for the future development of catalytic synergy.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Wilfred T. Diment, Gloria Rosetto, Noura Ezaz-Nikpay, Ryan W. F. Kerr, Charlotte K. Williams
Summary: The utilization of an iron(iii)/potassium(i) catalyst in ring-opening copolymerization of epoxides and anhydrides without additives/co-catalyst demonstrates high catalytic efficiency, loading tolerance, thermal stability, and selectivity. This catalyst exhibits unparalleled rates using terpene-derived monomers, resulting in bio-derived, amorphous polyesters with a high glass transition temperature (>100 degrees C), making them suitable for future applications as thermoplastics, block polymer adhesives, and elastomers.
Article
Materials Science, Multidisciplinary
Gi Byoung Hwang, Joe Stent, Sacha Noimark, Ki Joon Heo, Alexander J. Macrobert, Christopher W. M. Kay, Enrico Salvadori, Charlotte K. Williams, Sebastian D. Pike, Milo S. P. Shaffer, Elaine Allan, Ivan P. Parkin
Summary: In this study, a white light-activated bactericidal coating consisting of acrylic latex, ZnO NPs and CV was produced. The CV-dyed samples showed intrinsic bactericidal activity against S. aureus and the presence of ZnO NPs significantly enhanced the bactericidal activity. It is expected that this technique could be used to maintain low pathogen levels on hospital surfaces.
MATERIALS ADVANCES
(2023)
Article
Chemistry, Multidisciplinary
Thomas M. McGuire, Antoine Buchard, Charlotte Williams
Summary: A commercial Sn(II) catalyst combined with a commercial alcohol has been found to efficiently convert waste PLLA plastic into pure L-lactic acid at low temperatures. This catalyst system exhibits not only excellent catalytic activity and yield, but also significantly lower usage compared to previous catalysts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
