jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: Mizhi Xu | Banruo Huang | Haley K. Beech | Patrick T. Getty | Juan Manuel Urueña | Craig J. Hawker
Source: ACS Macro Letters (article, 2024-11-08)
Field: Chemistry — Organic Chemistry

Efficient Cross-Linking through C–H Bond Insertion of Unfunctionalized Commodity Materials Using Diazirine-Containing Polymers The synthesis and application of multifunctional diazirine-containing polymers for on-demand cross-linking of unfunctionalized commodity polymers through C-H bond insertion is demonstrated. While small-molecule diazirine cross-linkers have seen important applications such as plastic compatibilization and photopatterning, the high degree of functionalization of polymer-based diazirine cross-linkers offers promise for enhanced compatibility based on polymer blending and increased efficiency due to controllable multivalency. As a demonstrative example, unfunctionalized linear poly(<i>n</i>-butyl acrylate) (P<i>n</i>BA) can be cross-linked using various polymeric cross-linkers with diazirine contents as low as 0.8 wt % in 1 min under photochemical conditions. With gel fractions up to 95%, tunable rheological behavior is observed with increasing cross-linker loadings, consistent with a transition from entangled branched polymers to a cross-linked network. Moreover, the synthetic stability of the diazirine units can be exploited to prepare diazirine-containing polymers based on a variety of different backbones, from vinyl copolymers to poly(dimethylsiloxane) (PDMS), which allows successful photopatterning using a commercial 3D printer. Diazirine ; Polymer ; Polymer science ; Polymer chemistry ; Commodity ; Bond ; Materials science ; Chemistry ; Chemical engineering ; Organic chemistry ; Engineering ; Photochemistry ; Business Sulfur-Based Synthesis Techniques ; Nanomaterials for catalytic reactions ; Catalytic Cross-Coupling Reactions
Authors: Frédéric Grabowski | Fabian Fink | W. Sebastian Schier | Sven Soerensen | Alexander V. Petrunin | Walter Richtering | Sonja Herres‐Pawlis | Andrij Pich
Source: Advanced Functional Materials (article, 2024-05-20)
Field: Chemistry — Organic Chemistry

Catalyzed Henry Reaction by Compartmentalized Copper‐Pyrazolyl‐Complex Modified Microgels Abstract Compartmentalization of homogeneous catalysts enhances their catalytic performance and can even increase the selectivity. Microgels can serve as smart catalyst carrier systems offering the compartmentalization combined with good accessibility of the catalyst enabling the recyclability and re‐usability. Yet, the incorporation of coordination complexes into microgels has not been studied systematically, lacking in detailed insight in their structure and catalytic performance. Herein, microgels are synthesized with controlled number and localization of copper(II)‐pyrazolyl‐complexes. The catalytic activity of microgels in the Henry reactions is examined showing significantly higher yields compared to pure copper(II)‐pyrazolyl‐complexes. Furthermore, the localization of the copper(II)‐pyrazolyl‐complexes in the microgel core resulted in higher product yields than for microgel catalysts with copper(II) complexes in the shell. Microgel catalysts are demonstrated with copper(II) complexes that can be used in numerous reaction cycles, allow re‐loading of copper to recover catalytically active centers, and can be applicable in industrially‐relevant catalytic processes. Materials science ; Copper ; Chemical engineering ; Nitroaldol reaction ; Nanotechnology ; Catalysis ; Metallurgy ; Organic chemistry Nanomaterials for catalytic reactions ; Mesoporous Materials and Catalysis ; Porphyrin and Phthalocyanine Chemistry
Authors: Seung Hyeon Weon | Yuhyeon Na | Jiwoo Han | Jeong Woo Lee | Hyung Joo Kim | Saerom Park | Sang Hyun Lee
Source: Gels (article, 2024-03-16)
Field: Materials Science — Biomaterials

pH-Responsive Cellulose/Silk/Fe3O4 Hydrogel Microbeads Designed for Biomedical Applications In this study, cellulose/Fe<sub>3</sub>O<sub>4</sub> hydrogel microbeads were prepared through the sol-gel transition of a solvent-in-oil emulsion using various cellulose-dissolving solvents and soybean oil without surfactants. Particularly, 40% tetrabutylammonium hydroxide (TBAH) and 40% tetrabutylphosphonium hydroxide (TBPH) dissolved cellulose at room temperature and effectively dispersed Fe<sub>3</sub>O<sub>4</sub>, forming cellulose/Fe<sub>3</sub>O<sub>4</sub> microbeads with an average diameter of ~15 µm. Additionally, these solvents co-dissolved cellulose and silk, allowing for the manufacture of cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> hydrogel microbeads with altered surface characteristics. Owing to the negatively charged surface characteristics, the adsorption capacity of the cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> microbeads for the cationic dye crystal violet was >10 times higher than that of the cellulose/Fe<sub>3</sub>O<sub>4</sub> microbeads. When prepared with TBAH, the initial adsorption rate of bovine serum albumin (BSA) on the cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> microbeads was 18.1 times higher than that on the cellulose/Fe<sub>3</sub>O<sub>4</sub> microbeads. When preparing TBPH, the equilibrium adsorption capacity of the cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> microbeads for BSA (1.6 g/g) was 8.5 times higher than that of the cellulose/Fe<sub>3</sub>O<sub>4</sub> microbeads. The pH-dependent BSA release from the cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> microbeads prepared with TBPH revealed 6.1-fold slower initial desorption rates and 5.2-fold lower desorption amounts at pH 2.2 than those at pH 7.4. Cytotoxicity tests on the cellulose and cellulose/silk composites regenerated with TBAH and TBPH yielded nontoxic results. Therefore, cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> microbeads are considered suitable pH-responsive supports for orally administered protein pharmaceuticals. Cellulose ; Adsorption ; Dissolution ; Solvent ; Nanocellulose ; Hydroxide ; Materials science ; Chemistry ; Polymer chemistry ; Chemical engineering ; Nuclear chemistry ; Organic chemistry Silk-based biomaterials and applications ; Electrospun Nanofibers in Biomedical Applications ; Advanced Cellulose Research Studies
Authors: Ruggero Rossi | Daniele Martella | Camilla Parmeggiani | Max Hirschmann | Tiziana Fuoco
Source: ACS Applied Polymer Materials (article, 2024-01-11)
Field: Materials Science — Materials Chemistry

Photoswitches in Order: One-Pot Synthesis of Azobenzene Main-Chain and Segmented Copolymers Syntheses of multifunctional polymers aim to engineer a wide range of material properties by adjusting the composition and positioning of functional groups. While manifold syntheses of side-chain-functionalized polymers are known, synthetic protocols for main-chain-functionalized polymers are less common. This work describes a general one-pot strategy to prepare polymers containing multiple functional moieties in their main-chain, e.g., azobenzene units separated by variable oligomers. The polymerization proceeds in two steps, starting from a single azobenzene initiator and commercially available monomers (lactones and cyclic carbonates). Various main-chain-functionalized polymers were obtained with a predictable and adjustable ratio of monomer units (5–20) to photoswitchable azobenzene groups. The thermal properties of these polymers were analyzed and rationalized with regard to the parent polymers’ properties and the peculiarities arising from their segmented microstructure. Furthermore, the azobenzenes’ ability to undergo light-induced cis/trans-isomerization is confirmed. High isomerization yields of up to 90% were observed for the polymers in solution with a half-life of several days for the cis-isomers in solution. When irradiated as solid films, the azobenzenes still undergo isomerization, but the cis-isomers are less stable compared to the liquid state. Azobenzene ; Isomerization ; Polymer ; Monomer ; Copolymer ; Materials science ; Polymerization ; Polymer chemistry ; Side chain ; Photochemistry ; Chemistry ; Organic chemistry ; Catalysis ; Composite material Photochromic and Fluorescence Chemistry ; Advanced Polymer Synthesis and Characterization ; Supramolecular Self-Assembly in Materials
Authors: Cédric Gastaldi | Arnaud Gautier | Claude Forano | Virgil Hélaine | Christine Guérard‐Hélaine
Source: ChemCatChem (article, 2024-02-02)
Field: Chemistry — Inorganic Chemistry

Hybrid Catalysis in Concurrent Mode: How to Make Catalysts and Biocatalysts Compatible? Abstract For a long time, catalysis and biocatalysis seemed to be in competition until the organic chemist decided to synergize them for the better. However, their inherent differences presented such a challenge that most of the hybrid catalysis processes developed turned out to be sequential. Nevertheless, some processes have demonstrated that achieving the seemingly impossible was indeed feasible, by combining catalysts and biocatalysts in concurrent mode. This means having them operate under the same experimental conditions, in the presence of all reagents, from the start of the reaction cascade. The objective of this review is to illustrate how it became possible, drawing upon multidisciplinary fields such as organic and inorganic chemistry, chemo‐ and biocatalysis, to reconcile catalysts that are opposed by many parameters. Through a classification of encountered difficulties, organic chemists can swiftly identify methods to overcome them, creating a toolbox to develop new innovative processes. Biochemical engineering ; Biocatalysis ; Catalysis ; Chemistry ; Nanotechnology ; Toolbox ; Computer science ; Organic chemistry ; Ionic liquid ; Materials science ; Engineering Asymmetric Hydrogenation and Catalysis ; Chemical Synthesis and Analysis ; Catalysis for Biomass Conversion
Authors: T. F. Kouznetsova | Andrei Ivanets | Vladimir Prozorovich | Polina Shornikova | Lizaveta Kapysh | Qiang Tian | László Péter | László Trif | László Almásy
Source: Gels (article, 2024-02-06)
Field: Chemistry — Inorganic Chemistry

Design of Nickel-Containing Nanocomposites Based on Ordered Mesoporous Silica: Synthesis, Structure, and Methylene Blue Adsorption Mesoporous materials containing heteroelements have a huge potential for use as catalysts, exchangers, and adsorbents due to their tunable nanometer-sized pores and exceptionally large internal surfaces accessible to bulky organic molecules. In the present work, ordered mesoporous silica containing Ni atoms as active sites was synthesized by a new low-temperature method of condensation of silica precursors on a micellar template from aqueous solutions in the presence of nickel salt. The homogeneity of the resulting product was achieved by introducing ammonia and ammonium salt as a buffer to maintain a constant pH value. The obtained materials were characterized by nitrogen sorption, X-ray and neutron diffraction, scanning electron microscopy, infrared spectroscopy, and thermal analysis. Their morphology consists of polydisperse spherical particles 50-300 nm in size, with a hexagonally ordered channel structure, high specific surface area (A<sub>BET</sub> = 900-1200 m<sup>2</sup>/g), large pore volume (V<sub>p</sub> = 0.70-0.90 cm<sup>3</sup>/g), average mesopore diameter of about 3 nm, and narrow pore size distribution. Adsorption tests for methylene blue show sorption capacities reaching 39-42 mg/g at alkaline pH. The advantages of producing nickel silicates by this method, in contrast to precipitation from silicon alkoxides, are the low cost of reagents, fire safety, room-temperature processing, and the absence of specific problems associated with the use of ethanol as a solvent, as well as the absence of the inevitable capture of organic matter in the precipitation process. Methylene blue ; Adsorption ; Nickel ; Nanocomposite ; Mesoporous silica ; Methylene ; Materials science ; Chemical engineering ; Mesoporous material ; MCM-41 ; Inorganic chemistry ; Nuclear chemistry ; Chemistry ; Nanotechnology ; Organic chemistry ; Metallurgy ; Catalysis ; Molecular sieve Zeolite Catalysis and Synthesis ; Catalytic Processes in Materials Science ; Nanomaterials for catalytic reactions
Authors: Rupali A. Mendake | Pooja R. Hatwar | Ravindra L. Bakal | Shriyog V. Amalkar
Source: Journal of Drug Delivery and Therapeutics (article, 2024-08-15)
Field: Materials Science — Biomaterials

Review on Nanogel as a Novel Platform for Smart Drug Delivery System One of the most popular applications of nanotechnology in both topical and internal medicine administration to the body is nanogel technology. The materials comprising the nanoparticulate frameworks are less than 100 nm in a single measurement. The goal of this review paper is to provide a concise overview of the most recent developments in the nanogel medicine delivery framework with regard to drug loading and swelling. It categorises according to links (chemical and physical) and responding behaviour. This article is to give a broad overview of nanogels, their innovative use in many contexts, and current synthesis techniques. NGs use drugs for a variety of reasons, including diagnostics, gene targeting, organ targeting, and many more. Different pulmonary, nasal, transdermal, intra-ocular, oral, and parenteral routes can be used to give NGs. The primary goals of this review are to present broad details on NGs, their characteristics, multiple categories, medication targeting strategies, kinds of drug delivery systems, assessment techniques, and cutting-edge uses for NGs in depth. Keywords: Nanogel, DLS, CD, mechanism of drug release, classification, application Nanogel ; Drug delivery ; Computer science ; Nanotechnology ; Materials science Nanoparticle-Based Drug Delivery ; Advanced Drug Delivery Systems ; Hydrogels: synthesis, properties, applications
Authors: С.М. Самохвалова | Jean‐François Lutz | Ivan Coluzza
Source: Macromolecular Chemistry and Physics (article, 2024-10-15)
Field: Materials Science — Polymers and Plastics

Precision Design of Sequence‐Defined Polyurethanes: Exploring Controlled Folding Through Computational Design Abstract This study presents the exploration of sequence‐defined polyurethanes (PUs) as a new class of heteropolymers capable of precise conformational control. Utilizing molecular dynamics simulations, the folding behavior of polyurethane chains is investigated of varying lengths (11, 20, and 50 monomers) in both vacuum and aqueous environments. The simulations reveal that the heterogeneous chains systematically refold to approach the designed target structures better than non‐designed chains or chains with artificially disrupted hydrogen‐bond networks. The subsequent synthesis of an optimized 11‐mer sequence (P1) is achieved through solid‐phase chemistry, with thorough characterization via NMR, MS, and SEC confirming the accuracy of the predicted sequence and its controlled chain length. Solubility tests showed favorable results across multiple solvents, highlighting the versatility of the designed polymer. This research underscores the potential of sequence‐defined polyurethanes to emulate the structural and functional attributes of biological macromolecules, opening new pathways for their application in catalysis, drug delivery, and advanced material design. The findings illustrate a promising direction for the development of synthetic polymers with tailored properties, emphasizing the transformative impact of sequence control in polymer chemistry. Folding (DSP implementation) ; Sequence (biology) ; Polymer ; Macromolecule ; Monomer ; Materials science ; Polyurethane ; Chemistry ; Chain (unit) ; Hydrogen bond ; Nanotechnology ; Combinatorial chemistry ; Molecule ; Organic chemistry ; Engineering Polymer composites and self-healing ; Chemical Synthesis and Analysis ; Supramolecular Self-Assembly in Materials
Authors: Jonathan Becker
Source: ChemPlusChem (article, 2024-02-07)
Field: Materials Science — Electronic, Optical and Magnetic Materials

Understanding Cooperativity in Homo‐ and Heterometallic Complexes: From Basic Concepts to Design Cooperative effects have attracted considerable attention in recent years. These effects are ubiquitous in chemistry and biology and can govern interactions of proteins with other biomolecules, mechanisms of supramolecular recognition and polymerization, catalysis, assembly of compounds on surfaces, and physical properties such as magnetic, electronic or optical properties, e. g. Consequently, the understanding of cooperative effects can lead to a structure-property relation that can pave the way to future applications in various research areas; however, with regard to cooperative effects in homo- and heterometallic complexes, we still are at the beginning of understanding. Nevertheless, concepts to describe cooperativity of metal centers as well as methodologies to investigate and model these effects have emerged over the last years. This concept article gives an overview of these existing concepts, approaches, and strategies to understand cooperative effects in homo- and heterometallic complexes. Special emphasis is put on concepts to define cooperative effects, their quantification, as well as methods to investigate cooperative effects. Cooperativity ; Chemistry ; Nanotechnology ; Computational chemistry ; Materials science Magnetism in coordination complexes ; Lanthanide and Transition Metal Complexes ; Organometallic Complex Synthesis and Catalysis
Authors: Saptarshi Paul | Joshua Reyes-Morales | Kingshuk Roy | Jeffrey E. Dick
Source: ACS Nanoscience Au (article, 2024-04-18)
Field: Chemistry — Electrochemistry

Anodic Electrodeposition of IrO<sub><i>x</i></sub> Nanoparticles from Aqueous Nanodroplets Electrodeposition has been used for centuries to create new materials. However, synthetic platforms are still necessary to enrich a variety of nanomaterials that can be electrodeposited. For instance, IrO <sub><i>x</i></sub> is a popular material for the water oxidation reaction, but electrodeposition strategies for the controlled growth of IrO <sub><i>x</i></sub> nanoparticles are lacking. Here, we demonstrate the anodic electrodeposition of IrO <sub><i>x</i></sub> nanoparticles from aqueous nanodroplets. Field emission scanning electron microscopy (FESEM) and scanning transmission electron microscopy (STEM) images confirm the macro- and microstructure of the resulting nanoparticles. IrO <sub><i>x</i></sub> nanoparticles of 43 ± 10 nm in diameter were achieved. X-ray photoelectron spectroscopy (XPS) showed the presence of Ir(III) and Ir(IV) hydrated oxyhydroxide species. The synthesis of IrO <sub><i>x</i></sub> nanoparticles under anodic conditions using water nanodroplets expands the capabilities of our technique and provides a tunable platform for IrO <sub><i>x</i></sub> nanoparticle electrodeposition. Nanoparticle ; Aqueous solution ; Materials science ; Anode ; Nanotechnology ; Chemical engineering ; Chemistry ; Electrode ; Physical chemistry ; Engineering Electrochemical Analysis and Applications ; Electrocatalysts for Energy Conversion ; Advanced battery technologies research
Authors: Álvaro Miguel | Saúl Vallejos | José M. García | Miriam Trigo‐López
Source: European Polymer Journal (article, 2024-08-19)
Field: Materials Science — Polymers and Plastics

Boosting m-aramids performance with p-oriented aromatic amide side chains • High-performance m -aramid copolymers containing p -aramid side chains were obtained. • The aramid lateral chains were terminated with nitro groups. • Copolymers resulted in a 48% increase in the Young’s modulus compared to MPIA. • The performance of the new copolymers improved in upon exposure to hydrogen. • They can be applied as steel coatings in high-pressure hydrogen storage. This study aimed to enhance the mechanical properties of m -aramids by incorporating varying percentages of p -aramid side chains through copolymerization while ensuring solubility for practical applications. The mechanical performance of the resulting copolymers was compared with the commercial m -aramid, MPIA (poly( m -phenylene terephthalamide)). Notably, even with a 20% incorporation of p -aramid side chains, there was a substantial increase of 48% in Young’s modulus and 7% in tensile strength compared to MPIA. Additionally, the nitro group capping the p -aramid side chains demonstrated significant efficacy in enhancing the mechanical performance of the materials upon exposure to hydrogen. Specifically, there was an increase of more than 11% in Young’s modulus upon initial contact with hydrogen. This finding suggests potential applications in protective coatings for stainless steel used in high-pressure hydrogen storage environments. In such applications, exposure to hydrogen can accelerate embrittlement and limit operational lifespan, and coating with these materials can mitigate embrittlement and improve operational lifespan. Side chain ; Aramid ; Boosting (machine learning) ; Amide ; Chemistry ; Polymer chemistry ; Materials science ; Polymer science ; Combinatorics ; Mathematics ; Organic chemistry ; Computer science ; Artificial intelligence ; Polymer Synthesis and properties of polymers ; Chemical Synthesis and Analysis ; Dendrimers and Hyperbranched Polymers
Authors: Eliana Nope | Ángel G. Sathicq | José J. Martínez | Zeid A. ALOthman | Gustavo P. Romanelli | Elena Montejano Nares | Francisco Ivars‐Barceló | Juan Rubio‐Zuazo | Rafael Luque | Alina M. Balu
Source: Nanotechnology Reviews (article, 2024-01-01)
Field: Materials Science — Materials Chemistry

Revisiting hydrotalcite synthesis: Efficient combined mechanochemical/coprecipitation synthesis to design advanced tunable basic catalysts Abstract Hydrotalcite materials (HTs) were synthesized by a facile and swift combined mechanochemistry/coprecipitation approach, and their catalytic activity was evaluated and compared with conventionally synthesized hydrotalcites (co-precipitation method) in the Knoevenagel condensation between furfural and ethyl cyanoacetate/malononitrile. Characterization and catalytic activity results clearly demonstrate that the proposed combined mechanochemical/coprecipitation approach provides an improvement in crystallinity, morphology, tunable basicity, and textural properties (higher surface area and enhanced surface properties) as compared to HTs obtained via conventional coprecipitation methods. In addition, mechanochemically synthesized HTs largely improve catalytic activities, including conversion and product selectivity to Knoevenagel condensation products under solventless conditions, short reaction times, or reaction at room temperature as compared to conventional counterparts ( e.g. , 30–40 vs &gt; 99% product yields). Coprecipitation ; Knoevenagel condensation ; Hydrotalcite ; Malononitrile ; Catalysis ; Mechanosynthesis ; Crystallinity ; Materials science ; Chemical engineering ; Chemistry ; Organic chemistry ; Metallurgy ; Ball mill Layered Double Hydroxides Synthesis and Applications ; Mesoporous Materials and Catalysis