jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: Matthew J. Andrews | Ambre Carpentier | Alexandra M. Z. Slawin | David B. Cordes | Stuart A. Macgregor | Allan J. B. Watson
Source: ACS Catalysis (article, 2023-08-07)
Field: Chemistry — Organic Chemistry

Mechanism of Cu-Catalyzed Iododeboronation: A Description of Ligand-Enabled Transmetalation, Disproportionation, and Turnover in Cu-Mediated Oxidative Coupling Reactions We report a combined experimental and computational study of the mechanism of the Cu-catalyzed arylboronic acid iododeboronation reaction. A combination of structural and density functional theory (DFT) analyses has allowed determination of the identity of the reaction precatalyst with insight into each step of the catalytic cycle. Key findings include a rationale for ligand (phen) stoichiometry related to key turnover events-the ligand facilitates transmetalation via H-bonding to an organoboron boronate generated in situ and phen loss/gain is integral to the key oxidative events. These data provide a framework for understanding ligand effects on these key mechanistic processes, which underpin several classes of Cu-mediated oxidative coupling reactions. Transmetalation ; Disproportionation ; Catalytic cycle ; Ligand (biochemistry) ; Chemistry ; Catalysis ; Reductive elimination ; Oxidative phosphorylation ; Oxidative addition ; Density functional theory ; Oxidative coupling of methane ; Combinatorial chemistry ; Reaction mechanism ; Computational chemistry ; Photochemistry ; Organic chemistry ; Receptor Catalytic Cross-Coupling Reactions ; Catalytic C–H Functionalization Methods ; Organoboron and organosilicon chemistry
Authors: Marco Chino | Salvatore La Gatta | Linda Leone | Maria De Fenza | Angela Lombardi | Vincenzo Pavone | Ornella Maglio
Source: International Journal of Molecular Sciences (article, 2023-07-04)
Field: Materials Science — Materials Chemistry

Dye Decolorization by a Miniaturized Peroxidase Fe-MimochromeVI*a Oxidases and peroxidases have found application in the field of chlorine-free organic dye degradation in the paper, toothpaste, and detergent industries. Nevertheless, their widespread use is somehow hindered because of their cost, availability, and batch-to-batch reproducibility. Here, we report the catalytic proficiency of a miniaturized synthetic peroxidase, Fe-Mimochrome VI*a, in the decolorization of four organic dyes, as representatives of either the heterocyclic or triarylmethane class of dyes. Fe-Mimochrome VI*a performed over 130 turnovers in less than five minutes in an aqueous buffer at a neutral pH under mild conditions. Peroxidase ; Chemistry ; Aqueous solution ; Degradation (telecommunications) ; Chlorine ; Toothpaste ; Nuclear chemistry ; Chromatography ; Organic chemistry ; Enzyme Advanced Nanomaterials in Catalysis ; Enzyme-mediated dye degradation ; Chromium effects and bioremediation
Authors: Changfeng Yin | Jiaxing Du | Bogdan Olenyuk | Peter J. Stang | Yan Sun
Source: Inorganics (article, 2023-01-22)
Field: Chemistry — Inorganic Chemistry

The Applications of Metallacycles and Metallacages Metallacycles and metallacages constitute a class of coordination compounds composed of metal ions and organic ligands. Because of their precise stoichiometry, the flexibility and viability of design, metallacycles and metallacages have attracted considerable attention as supramolecular assemblies. Various two-dimensional polygons, three-dimensional polyhedra, and other nanoscale materials have been constructed and applied. The highly diverse structures, sizes, and shapes endow metallacycles and metallacages with unique physical and chemical properties and make them suitable for various applications such as encapsulation, separation, catalysis, and biological science. Herein, we review the recent developments in various metallacycles and metallacages in different fields. The text highlights biomedical applications involving molecular recognition and binding, antibacterial activity, and especially cancer diagnosis and treatment, including imaging, chemotherapy, PDT, and PTT. Supramolecular chemistry ; Nanotechnology ; Nanoscopic scale ; Materials science ; Flexibility (engineering) ; Stoichiometry ; Chemistry ; Molecule ; Physical chemistry ; Organic chemistry ; Mathematics Metal-Organic Frameworks: Synthesis and Applications ; Nanoplatforms for cancer theranostics ; Supramolecular Chemistry and Complexes
Authors: Uğur Tutar | Cem Çeli̇k | Elvan Üstün | Namık Özdemir | Neslihan Şahin | David Sémeril | Nevın Gürbüz | İsmaıl Özdemır
Source: Inorganics (article, 2023-09-27)
Field: Chemistry — Organic Chemistry

Benzimidazol-2-ylidene Silver Complexes: Synthesis, Characterization, Antimicrobial and Antibiofilm Activities, Molecular Docking and Theoretical Investigations Five silver(I) complexes, namely chloro[1-methallyl-3-benzyl)benzimidazol-2-ylidene] silver (6), chloro[1-methallyl-3-(2,3,5,6-tetramethylbenzyl)benzimidazol-2-ylidene]silver (7), chloro[1-methallyl-3-(3,4,5-trimethoxylbenzyl)benzimidazol-2-ylidene]silver (8), chloro[1-methallyl- 3-(naphthylmethyl)benzimidazol-2-ylidene]silver (9), and chloro [1-methallyl-3-(anthracen-9-yl- methyl)benzimidazol-2-ylidene]silver (10), were prepared starting from their corresponding benzimidazolium salts and silver oxide in 71–81% yields. A single-crystal X-ray structure of 7 was determined. These five Ag-NHC complexes were evaluated for their antimicrobial and biofilm formation inhibition properties. Complex 10 exhibited high antimicrobial activities comparable to those obtained with standard drugs such as Fluconazole in contact with Staphylococcus aureus, Enterococcus faecalis, Escherichia coli, Acinetobacter baumannii, and Candida albicans. The latter complex has been shown to be very efficient in antibiofilm activity, with 92.9% biofilm inhibition at 1.9 μg/mL on Escherichia coli. Additionally, the molecules were optimized with DFT-based computational methods for obtaining insight into the structure/reactivity relations through the relative energies of the frontier orbitals. The optimized molecules were also analyzed by molecular docking method against DNA gyrase of Escherichia coli and CYP51 from Candida albicans. Escherichia coli ; Docking (animal) ; Candida albicans ; Chemistry ; Antimicrobial ; Enterococcus faecalis ; Biofilm ; Stereochemistry ; Microbiology ; Organic chemistry ; Bacteria ; Biochemistry ; Biology N-Heterocyclic Carbenes in Organic and Inorganic Chemistry ; Catalytic Cross-Coupling Reactions ; Catalytic Alkyne Reactions
Authors: Xia Li | Debobroto Sensharma | Varvara I. Nikolayenko | Shaza Darwish | Andrey A. Bezrukov | Naveen Kumar | Wansheng Liu | Xiang‐Jing Kong | Zhenjie Zhang | Michael J. Zaworotko
Source: Chemistry of Materials (article, 2023-01-10)
Field: Chemistry — Inorganic Chemistry

Structural Phase Transformations Induced by Guest Molecules in a Nickel-Based 2D Square Lattice Coordination Network Herein, we report the crystal structure and guest binding properties of a new two-dimensional (2D) square lattice (<b>sql</b>) topology coordination network, <b>sql-(azpy)(pdia)-Ni</b>, which is comprised of two linker ligands with diazene (azo) moieties, (<i>E</i>)-1,2-di(pyridin-4-yl)diazene(azpy) and (<i>E</i>)-5-(phenyldiazenyl)isophthallate(pdia). <b>sql-(azpy)(pdia)-Ni</b> underwent guest-induced switching between a closed (nonporous) <b>β</b> phase and several open (porous) <b>α</b> phases, but unlike the clay-like layer expansion to distinct phases previously reported in switching <b>sql</b> networks, a continuum of phases was formed. In effect, <b>sql-(azpy)(pdia)-Ni</b> exhibited elastic-like properties induced by adaptive guest binding. Single-crystal X-ray diffraction (SCXRD) studies of the <b>α</b> phases revealed that the structural transformations were enabled by the pendant phenyldiazenyl moiety on the pdia<sup>2-</sup> ligand. This moiety functioned as a type of hinge to enable parallel slippage of layers and interlayer expansion for the following guests: <i>N</i>,<i>N</i>-dimethylformamide, water, dichloromethane, <i>para</i>-xylene, and ethylbenzene. The slippage angle (interplanar distances) ranged from 54.133° (4.442 Å) in the <b>β</b> phase to 69.497° (5.492 Å) in the ethylbenzene-included phase. Insight into the accompanying phase transformations was also gained from variable temperature powder XRD studies. Dynamic water vapor sorption studies revealed a stepped isotherm with little hysteresis that was reversible for at least 100 cycles. The isotherm step occurred at ca. 50% relative humidity (RH), the optimal RH value for humidity control. Crystallography ; Chemistry ; Moiety ; Materials science ; Crystal structure ; Topology (electrical circuits) ; Stereochemistry Metal-Organic Frameworks: Synthesis and Applications ; Supramolecular Self-Assembly in Materials ; Crystallography and molecular interactions
Authors: Michal Trachta | Ota Bludský | Jan Vaculík | Roman Bulánek | Miroslav Rubeš
Source: Scientific Reports (article, 2023-07-31)
Field: Chemistry — Inorganic Chemistry

Investigation of Brønsted acidity in zeolites through adsorbates with diverse proton affinities Understanding the adsorption behavior of base probes in aluminosilicates and its relationship to the intrinsic acidity of Brønsted acid sites (BAS) is essential for the catalytic applications of these materials. In this study, we investigated the adsorption properties of base probe molecules with varying proton affinities (acetonitrile, acetone, formamide, and ammonia) within six different aluminosilicate frameworks (FAU, CHA, IFR, MOR, FER, and TON). An important objective was to propose a robust criterion for evaluating the intrinsic BAS acidity (i.e., state of BAS deprotonation). Based on the bond order conservation principle, the changes in the covalent bond between the aluminum and oxygen carrying the proton provide a good description of the BAS deprotonation state. The ammonia and formamide adsorption cause BAS deprotonation and cannot be used to assess intrinsic BAS acidity. The transition from ion-pair formation, specifically conjugated acid/base interaction, in formamide to strong hydrogen bonding in acetone occurs within a narrow range of base proton affinities (812-822 kJ mol<sup>-1</sup>). The adsorption of acetonitrile results in the formation of hydrogen-bonded complexes, which exhibit a deprotonation state that follows a similar trend to the deprotonation induced by acetone. This allows for a semi-quantitative comparison of the acidity strengths of BAS within and between the different aluminosilicate frameworks. Deprotonation ; Protonation ; Chemistry ; Formamide ; Hydrogen bond ; Aluminosilicate ; Proton affinity ; Inorganic chemistry ; Adsorption ; Affinities ; Acetonitrile ; Catalysis ; Molecule ; Physical chemistry ; Organic chemistry ; Stereochemistry ; Ion Zeolite Catalysis and Synthesis ; Chemical Synthesis and Characterization ; Metal-Organic Frameworks: Synthesis and Applications
Authors: Edoardo Miravalle | Pierangiola Bracco | Valentina Brunella | Claudia Barolo | Marco Zanetti
Source: Polymers (review, 2023-09-15)
Field: Materials Science — Polymers and Plastics

Improving Sustainability through Covalent Adaptable Networks in the Recycling of Polyurethane Plastics The global plastic waste problem has created an urgent need for the development of more sustainable materials and recycling processes. Polyurethane (PU) plastics, which represent 5.5% of globally produced plastics, are particularly challenging to recycle owing to their crosslinked structure. Covalent adaptable networks (CANs) based on dynamic covalent bonds have emerged as a promising solution for recycling PU waste. CANs enable the production of thermoset polymers that can be recycled using methods that are traditionally reserved for thermoplastic polymers. Reprocessing using hot-pressing techniques, in particular, proved to be more suited for the class of polyurethanes, allowing for the efficient recycling of PU materials. This Review paper explores the potential of CANs for improving the sustainability of PU recycling processes by examining different types of PU-CANs, bond types, and fillers that can be used to optimise the recycling efficiency. The paper concludes that further research is needed to develop more cost-effective and industrial-friendly techniques for recycling PU-CANs, as they can significantly contribute to sustainable development by creating recyclable thermoset polymers. Thermosetting polymer ; Polyurethane ; Sustainability ; Materials science ; Plastic waste ; Covalent bond ; Polymer ; Thermoplastic ; Plastics industry ; Process engineering ; Waste management ; Polymer science ; Manufacturing engineering ; Composite material ; Engineering ; Organic chemistry ; Chemistry Polymer composites and self-healing ; Synthetic Organic Chemistry Methods ; biodegradable polymer synthesis and properties
Authors: Charlotte N. Stindt | Stefano Crespi | Ryojun Toyoda | Michiel Hilbers | Johan Kemmink | Pieter van der Meulen | Wybren Jan Buma | Ben L. Feringa
Source: Chem (article, 2023-07-11)
Field: Chemistry — Organic Chemistry

Activating a light-driven molecular motor by metal complexation Ligand (biochemistry) ; Molecular motor ; Molecular machine ; Metal ; Rotation around a fixed axis ; Nanotechnology ; Molecular switch ; Chemistry ; Function (biology) ; Materials science ; Chemical physics ; Molecule ; Physics ; Receptor Supramolecular Chemistry and Complexes ; Porphyrin and Phthalocyanine Chemistry ; Magnetism in coordination complexes
Authors: Shuaishuai Zhu | Maoji Zhao | Hongru Zhou | Yingfeng Wen | Yong Wang | Yonggui Liao | Xingping Zhou | Xiaolin Xie
Source: Nature Communications (article, 2023-03-23)
Field: Materials Science — Polymers and Plastics

One-pot synthesis of hyperbranched polymers via visible light regulated switchable catalysis Switchable catalysis promises exceptional efficiency in synthesizing polymers with ever-increasing structural complexity. However, current achievements in such attempts are limited to constructing linear block copolymers. Here we report a visible light regulated switchable catalytic system capable of synthesizing hyperbranched polymers in a one-pot/two-stage procedure with commercial glycidyl acrylate (GA) as a heterofunctional monomer. Using (salen)Co<sup>III</sup>Cl (1) as the catalyst, the ring-opening reaction under a carbon monoxide atmosphere occurs with high regioselectivity (>99% at the methylene position), providing an alkoxycarbonyl cobalt acrylate intermediate (2a) during the first stage. Upon exposure to light, the reaction enters the second stage, wherein 2a serves as a polymerizable initiator for organometallic-mediated radical self-condensing vinyl polymerization (OMR-SCVP). Given the organocobalt chain-end functionality of the resulting hyperbranched poly(glycidyl acrylate) (hb-PGA), a further chain extension process gives access to a core-shell copolymer with brush-on-hyperbranched arm architecture. Notably, the post-modification with 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) affords a metal-free hb-PGA that simultaneously improves the toughness and glass transition temperature of epoxy thermosets, while maintaining their storage modulus. Acrylate ; Copolymer ; Materials science ; Monomer ; Polymer chemistry ; Polymerization ; Catalysis ; Polymer ; Glycidyl methacrylate ; Chemistry ; Organic chemistry ; Composite material Dendrimers and Hyperbranched Polymers ; Advanced Polymer Synthesis and Characterization ; Synthetic Organic Chemistry Methods
Authors: Jie Li | Yushan Li | Yiyi Lu | Yuke Wang | Yunjie Guo | Wentian Shi
Source: Biomimetics (review, 2023-01-15)
Field: Materials Science — Surfaces, Coatings and Films

Preparation of 2D Materials and Their Application in Oil–Water Separation The problems of environmental pollution are increasingly severe. Among them, industrial wastewater is one of the primary sources of pollution, so it is essential to deal with wastewater, especially oil and water mixtures. At present, biomimetic materials with special wettability have been proven to be effective in oil-water separation. Compared with three-dimensional (3D) materials, two-dimensional (2D) materials show unique advantages in the preparation of special wettable materials due to their high specific surface area, high porosity, controlled structure, and rich functional group rich on the surface. In this review, we first introduce oil-water mixtures and the common oil-water separation mechanism. Then, the research progress of 2D materials in oil-water separation is presented, including but not limited to their structure, types, preparation principles, and methods. In addition, it is still impossible to prepare 2D materials with large sizes because they are powder-like, which greatly limits the application in oil-water separation. Therefore, we provide here a review of several ways to transform 2D materials into 3D materials. In the end, the challenges encountered by 2D materials in separating oil-water are also clarified to promote future applications. Pollution ; Porosity ; Oil pollution ; Wetting ; Wastewater ; Materials science ; Environmental science ; Water pollution ; Process engineering ; Petroleum engineering ; Environmental engineering ; Environmental chemistry ; Geology ; Chemistry ; Composite material ; Engineering Surface Modification and Superhydrophobicity ; Covalent Organic Framework Applications ; Advanced Sensor and Energy Harvesting Materials
Authors: Xiaxuan Ran | Yunzhuo Qu | Yijie Wang | Bowen Cui | Yushan Shen | Yuanzhe Li
Source: Journal of Composites Science (article, 2023-10-04)
Field: Materials Science — Biomaterials

Enhanced UV-Blocking Capabilities of Polylactic Acid Derived from Renewable Resources for Food and Drug Packaging: A Mini-Review Plastic materials have revolutionized modern life, particularly in the domain of food packaging, owing to their versatility, lightweight nature, and ease of processing. However, the environmental ramifications of non-degradable plastics have raised concerns. Polylactic acid (PLA), derived from renewable sources, represents a sustainable alternative due to its biodegradability and exceptional barrier, mechanical, and safety properties. Nevertheless, the high UV transmittance of PLA limits its use for photosensitive food and pharmaceutical packaging, where UV radiation can lead to nutritional loss and spoilage. Various methods have been explored to enhance the UV-blocking capabilities of PLA, including the integration of inorganic nanoparticles and surface coatings. Despite advancements, these approaches often compromise the inherent transparency of PLA. Incorporating large conjugated groups can maintain transparency but introduces additional challenges. This paper reviews modification methods to enhance PLA’s UV-barrier properties and anticipates its expanded utility in food and drug packaging, promoting UV resistance and diversifying PLA’s applications. Polylactic acid ; Food packaging ; Transparency (behavior) ; Materials science ; Active packaging ; Nanotechnology ; Biochemical engineering ; Polymer ; Chemistry ; Computer science ; Engineering ; Composite material ; Food science biodegradable polymer synthesis and properties ; Microplastics and Plastic Pollution ; Additive Manufacturing and 3D Printing Technologies
Authors: Inna A. Abdulaeva | Kirill P. Birin | Rémi Chassagnon | Alla Bessmertnykh‐Lemeune
Source: Catalysts (article, 2023-02-13)
Field: Materials Science — Materials Chemistry

Hybrid Materials Based on Imidazo[4,5-b]porphyrins for Catalytic Oxidation of Sulfides Heterogenized metalloporphyrin catalysts for oxidation reactions are extensively explored to improve chemical production. In this work, manganese meso-tetraarylporphyrins were immobilized on hydrated mesoporous titanium dioxide (SBET = 705 m2 g−1) through carboxylate or phosphonate anchoring groups separated from the macrocycle by the 2-arylimidazole linker fused across one of the pyrrolic rings of the macrocycle. The element composition of two mesoporous hybrid materials thus obtained were investigated and the integrity of the immobilized complexes was shown by different physicochemical methods. Finally, the catalytic efficiency of the more stable material Mn(TMPIP)/TiO2 with the phosphonate anchor was evaluated in the selective oxidation of sulfides to sulfoxides by molecular oxygen in the presence of isobutyraldehyde (IBA). The heterogenized complex has shown excellent catalytic activity exhibiting a turnover (TON) of ~1100 in a single catalytic run of the sulfoxidation of thioanisole. The catalyst was successfully reused in seven consecutive catalytic cycles. Thioanisole ; Isobutyraldehyde ; Catalysis ; Phosphonate ; Chemistry ; Manganese ; Mesoporous material ; Catalytic oxidation ; Carboxylate ; Combinatorial chemistry ; Bifunctional ; Hybrid material ; Polymer chemistry ; Organic chemistry Porphyrin and Phthalocyanine Chemistry ; Oxidative Organic Chemistry Reactions ; Covalent Organic Framework Applications
Authors: Shaotian Zhang | Dafu Wei | Xiang Xu | Yong Guan
Source: Coatings (article, 2023-06-17)
Field: Materials Science — Biomaterials

Transparent, High-Strength, and Antimicrobial Polyvinyl Alcohol/Boric Acid/Poly Hexamethylene Guanidine Hydrochloride Films It is still crucial to improve the mechanical characteristics of polyvinyl alcohol (PVA) films without resorting to chemical cross-linking. In this study, boric acid (BA) was used to enhance the mechanical characteristics of PVA films while maintaining their excellent transparency and biodegradability. The hydrogen bond interaction between PVA and BA resulted in a 70% increase in tensile strength (from 48.5 to 82.1 MPa) and a 46% increase in elongation at break (from 150 to 220%). To introduce antibacterial properties, polyhexamethylene guanidine hydrochloride (PHMG) was incorporated into PVA/BA composite films resulting in PVA/BA/PHMG composite films. The PVA/BA/PHMG films exhibited 99.99% bacterial inhibition against Escherichia coli and Staphylococcus aureus with negligible leaching of PHMG. The PVA/BA/PHMG films maintained a tensile strength of 75.3 MPa and an elongation at a break of 208%. These improved mechanical and antimicrobial properties make PVA/BA and PVA/BA/PHMG films promising for applications in food and medicinal packaging. Polyvinyl alcohol ; Ultimate tensile strength ; Materials science ; Boric acid ; Composite number ; Composite material ; Chemical engineering ; Antimicrobial ; Vinyl alcohol ; Polymer ; Chemistry ; Organic chemistry biodegradable polymer synthesis and properties ; Electrospun Nanofibers in Biomedical Applications ; Nanocomposite Films for Food Packaging